Catalyst compositions and applications thereof

ABSTRACT

In one aspect, structural catalyst bodies comprising one or more gradients of catalytic material are provided herein. In some embodiments, a structural catalyst body described herein comprises an inner partition wall having a first surface and a second surface opposite the first surface, the inner partition wall having a gradient of catalytic material along the width of the inner partition wall.

RELATED APPLICATION DATA

The present application hereby claims priority to U.S. ProvisionalPatent Application Ser. No. 61/371,971, filed Aug. 9, 2010 and to U.S.Provisional Patent Application Ser. No. 61/371,948, filed Aug. 9, 2010,each of which is incorporated herein by reference in its entirety.

FIELD

The present invention relates to catalyst compositions and, inparticular, to catalyst structures for use in industrial or commercialapplications.

BACKGROUND

The role nitrogen oxides in the formation of acid rain, troposphericozone and other environmental hazards has resulted in the imposition ofstrict standards limiting the discharges of these chemical species. Tomeet these standards, it is generally necessary to remove at least partof these oxides present in the exhaust gases from stationary or mobilecombustion sources.

Denitration or selective catalytic reduction (SCR) technology iscommonly applied to combustion-derived flue gases for removal ofnitrogen oxides. The denitration reaction comprises the reaction ofnitrogen oxide species in the gases, such as nitrogen oxide (NO) ornitrogen dioxide (NO₂), with a nitrogen containing reductant, such asammonia or urea, resulting in the production of diatomic nitrogen (N₂)and water.

In addition to nitrogen oxides, sulfur dioxide (SO₂) is a chemicalspecies often present in combustion-flue gases that causes environmentalconcern. Sulfur dioxide present in fossil fuel combustion flue-gases ispartly oxidized to sulfur trioxide (SO₃) which reacts with water to formsulfuric acid. The formation of sulfuric acid from the oxidation ofsulfur dioxide in combustion flue-gases can increase corrosion problemsin downstream equipment, can increase power costs associated with airpre-heaters due to the increased temperature required to keep theacid-containing flue-gas above its dew point, and can cause increasedopacity in the stack gases emitted to the atmosphere.

Catalyst systems for the removal of nitrogen oxides can increase theamount of sulfur dioxide oxidation since catalytic material utilized inselective catalytic reduction can additionally effectuate the oxidationof sulfur dioxide. As a result, the reduction in the nitrogen oxidecontent of a combustion flue-gas can have an undesirable side-effect ofincreasing SO₃ formation in the combustion flue-gas.

SUMMARY

In one aspect, catalyst bodies are described herein which, in someembodiments, display heterogeneous distributions of catalytic material.In some embodiments, catalyst bodies described herein are operable forthe selective catalytic reduction of nitrogen oxides in a flue gasstream. Structural catalyst bodies described herein, in someembodiments, can reduce SO₂ oxidation during nitrogen oxide removal froma flue gas stream.

In some embodiments, a structural catalyst body described hereincomprises at least one inner partition wall comprising first surface anda second surface opposite the first surface, the inner partition wallhaving a gradient of a first catalytic material along a width of thefirst surface. In some embodiments, the first catalytic material of thegradient decreases in amount at the periphery of the width of the firstsurface. In some embodiments, the first catalytic material of thegradient increases in amount along a central region of the width of thefirst surface. In some embodiments, a gradient of a first catalyticmaterial along the width of the first surface of the inner partitionwall has a profile symmetrical or substantially symmetrical about themidpoint of the profile.

A structural catalyst body, in some embodiments, further comprises agradient of the first catalytic material along a width of the secondsurface. In some embodiments, the first catalytic material of thegradient decreases in amount at the periphery of the width of the secondsurface. The first catalytic material of the gradient, in someembodiments, increases in amount along a central region of the width ofthe second surface. In some embodiments, the gradient profile of thefirst catalytic material along the width of the second surface issymmetrical or substantially symmetrical to the gradient profile of thefirst catalytic material along the width of the first surface.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of the first catalytic material along a length ofthe first surface of the inner partition wall. A gradient of the firstcatalytic material along the length of the first surface of the innerpartition wall, in some embodiments, comprises a greater amount of thefirst catalytic material at a first end of the inner partition wall incomparison with an amount of the first catalytic material at a secondend of the inner partition wall, the second end opposite the first end.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of the first catalytic material along a length ofthe second surface of the inner partition wall. A gradient of the firstcatalytic material along the length of the second surface of the innerpartition wall, in some embodiments, comprises a greater amount of thefirst catalytic material at a first end of the inner partition wall incomparison with an amount of the first catalytic material at a secondend of the inner partition wall, the second end opposite the first end.In some embodiments, the gradient profile of the first catalyticmaterial along the length of the second surface of the inner partitionwall is symmetrical or substantially symmetrical to the gradient profileof the first catalytic material along the length of the first surface ofthe inner partition wall.

In some embodiments, the first end of the inner partition wallcorresponds to the fluid stream inlet side of the structural catalystbody, and the second end corresponds to the fluid stream outlet side ofthe structural catalyst body. In some embodiments, the first end of theinner partition wall corresponds to the fluid stream outlet side of thestructural catalyst body, and the second end corresponds to the fluidstream inlet of the structural catalyst body.

In some embodiments, a structural catalyst body described hereincomprises a gradient of bulk first catalytic material along a width ofat least one inner partition wall. In some embodiments, bulk firstcatalytic material of the gradient decreases in concentration at theperiphery of the width of the inner partition wall. In some embodiments,bulk first catalytic material increases in concentration along a centralregion of the width of the inner partition wall. In some embodiments, agradient of bulk first catalytic material along the width of the innerpartition wall has a profile symmetrical or substantially symmetricalabout the midpoint of the profile.

In some embodiments, a structural catalyst body described hereincomprises a gradient of bulk first catalytic material along a length ofat least one inner partition wall. In some embodiments, a gradient ofbulk first catalytic material along a length of an inner partition wallcomprises a greater concentration of the bulk first catalytic materialat a first end of the inner partition wall in comparison with anconcentration of the bulk first catalytic material at a second end ofthe inner partition wall, the second end opposite the first end. Asdescribed herein, in some embodiments, the first end of the innerpartition wall corresponds to the fluid stream inlet side of thestructural catalyst body, and the second end corresponds to the fluidstream outlet side of the structural catalyst body. In some embodiments,the first end of the inner partition wall corresponds to the fluidstream outlet side of the structural catalyst body, and the second endcorresponds to the fluid stream inlet of the structural catalyst body.

A structural catalyst body described herein, in some embodiments,further comprises at least one additional inner partition wallcomprising one or more gradients of the first catalytic materialdescribed herein for an inner partition wall. In some embodiments, theat least one additional inner partition wall comprises a first surfaceand a second surface and a gradient of the first catalytic materialalong a width of the first surface. In some embodiments, the at leastone additional inner partition wall further comprises a gradient of thefirst catalytic material along a width of the second surface.

Moreover, in some embodiments, the at least one additional innerpartition wall comprises a gradient of bulk first catalytic materialalong a width of the additional inner partition wall. In someembodiments, the at least one additional inner partition wall comprisesa gradient of bulk first catalytic material along a length of the innerpartition wall.

The at least one additional inner partition wall, in some embodiments,comprises a gradient of the first catalytic material along the length ofthe first surface and/or second surface.

In some embodiments, the at least one additional inner partition wallcomprises a plurality of additional inner partition walls such thatgreater than about 50 percent of the inner partition walls of thestructural catalyst body comprise one or more gradients of the firstcatalytic material described herein. In some embodiments, greater thanabout 70 or greater than about 90 percent of the inner partition wallsof the structural catalyst body comprise one or more gradients of thefirst catalytic material described herein. In some embodiments, greaterthan about 95 percent of the inner partition walls of the structuralcatalyst body comprise one or more gradients of the first catalyticmaterial described herein.

In some embodiments, inner partition walls of a structural catalyst bodydescribed herein intersect to form one or more centerposts. In someembodiments, a structural catalyst body described herein comprises agradient of bulk first catalytic material between a centerpost and atleast one inner partition wall connected to the centerpost. In someembodiments, for example, the at least one inner partition wallcomprises a greater concentration of a bulk first catalytic materialthan the centerpost. In some embodiments, a structural catalyst bodydescribed herein comprises a gradient of bulk first catalytic materialbetween a centerpost and a plurality of inner partition walls connectedto the centerpost. In some embodiments, each of the inner partitionwalls connected to the centerpost comprises a greater concentration of abulk first catalytic material than the centerpost.

In some embodiments, inner partition walls define a plurality of flowchannels or cells which extend through the structural catalyst body. Insome embodiments, inner partition walls are at least partiallysurrounded by an outer peripheral wall or structure. In someembodiments, an outer peripheral wall is continuous or integral with oneor more inner partition walls, such as in some honeycomb-like structuralcatalyst bodies. In some embodiments, an outer peripheral wall is partof a containment structure in which the inner partition walls aredisposed, such as in the arrangement of plate catalyst elements orcorrugated catalyst elements in a containment structure.

In some embodiments wherein the outer peripheral wall comprises bulkfirst catalytic material, inner partition walls of a structural catalystbody comprise more bulk first catalytic material than the outerperipheral wall. Moreover, in some embodiments, an interior surface ofan outer peripheral wall comprises one or more gradients of the firstcatalytic material described herein for an inner partition wall. In someembodiments, outer surfaces of an outer peripheral wall do not displayone or more gradients of the first catalytic material described herein.In some embodiments, an interior surface of an outer peripheral wallcomprises a greater amount of first catalytic material than an exteriorsurface of the inner partition wall.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of a second catalytic material along the width ofthe first surface of at least one inner partition wall. In someembodiments, a gradient of a second catalytic material along the widthof the first surface of at least one inner partition wall can have anyof the properties recited herein for a gradient of the first catalyticmaterial along the width of the first surface of an inner partitionwall.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of a second catalytic material along the width ofthe second surface of at least one inner partition wall. In someembodiments, a gradient of a second catalytic material along the widthof the second surface of the inner partition wall can have any of theproperties recited herein for a gradient of the first catalytic materialalong the width of the second surface of an inner partition wall.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of second catalytic material along a length of thefirst surface of the at least one inner partition wall. In someembodiments, a gradient of at a second catalytic material along a lengthof the first surface of the inner partition wall can have any of theproperties recited herein for a gradient of the first catalytic materialalong a length of the first surface of the inner partition wall.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of a second catalytic material along a length ofthe second surface of at least one inner partition wall. In someembodiments, a gradient of a second catalytic material along a length ofthe second surface of the inner partition wall can have any of theproperties recited herein for a gradient of the first catalytic materialalong a length of the second surface of an inner partition wall.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of a bulk second catalytic material along the widthof at least one inner partition wall. In some embodiments, a gradient ofa bulk second catalytic material can have any of the properties recitedherein for a gradient of a bulk first catalytic material along a widthof the inner partition wall.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of a bulk second catalytic material along a lengthof at least one inner partition wall. In some embodiments, a gradient ofa bulk second catalytic material along a length of an inner partitionwall can have any of the properties recited herein for a gradient of abulk first catalytic material along a length of an inner partition wall.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of a second catalytic material along the width ofthe first surface of at least one additional inner partition wall. Insome embodiments, a gradient of a second catalytic material along thewidth of the first surface of at least one additional inner partitionwall can have any of the properties recited herein for a gradient of afirst catalytic material along the width of the first surface of aninner partition wall.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of a second catalytic material along the width ofthe second surface of at least one additional inner partition wall. Insome embodiments, a gradient of a second catalytic material along thewidth of the second surface of at least one additional inner partitionwall can have any of the properties recited herein for a gradient of afirst catalytic material along the width of the second surface of aninner partition wall.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of a bulk second catalytic material along the widthof at least one additional inner partition wall. In some embodiments, agradient of bulk second catalytic material along the width of at leastone additional inner partition wall can have any of the propertiesrecited herein for a gradient of a bulk first catalytic material alongthe width of an inner partition wall.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of a bulk second catalytic material along a lengthof at least one additional inner partition wall. In some embodiments, agradient of a bulk second catalytic material along the length of atleast one additional inner partition wall can have any of the propertiesrecited herein for a gradient of a bulk first catalytic material along alength of an inner partition wall.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of a second catalytic material along a length ofthe first and/or second surface of at least one additional innerpartition wall. In some embodiments, a gradient of a second catalyticmaterial along a length of the first and/or second surface of at leastone additional inner partition wall can have any of the propertiesrecited herein for a gradient of the first catalytic material along alength of the first/and or second surface of an inner partition wall.

In some embodiments, a structural catalyst body described hereincomprises a gradient of a bulk second catalytic material between acenterpost and at least one inner partition wall connected to thecenterpost. In some embodiments, for example, at least one innerpartition wall comprises a greater concentration of a bulk secondcatalytic material than the centerpost. In some embodiments, astructural catalyst body described herein comprises a gradient of a bulksecond catalytic material between a centerpost and a plurality of innerpartition walls connected to the centerpost. In some embodiments, eachof the inner partition walls connected to the centerpost comprises agreater concentration of a bulk second catalytic material than thecenterpost.

Moreover, in some embodiments, an outer peripheral wall furthercomprises a bulk second catalytic material, wherein inner partitionwalls of the structural catalyst body comprise a greater amount of thebulk second catalytic material than the outer peripheral wall. In someembodiments, an interior surface of an outer peripheral wall furthercomprises one or more gradients of the second catalytic materialdescribed herein for an inner partition wall.

In some embodiments, a structural catalyst body further comprises agradient of at least one additional catalytic material. A gradient of atleast one additional catalytic material can comprise any constructionand/or location in a structural catalyst body described herein for agradient of a first catalytic material or a second catalytic material.

Structural catalyst bodies described herein, in some embodiments,comprise virgin structural catalyst bodies. In some embodiments,structural catalyst bodies described herein comprise used or regeneratedstructural catalyst bodies. In some embodiments, structural catalystbodies described herein comprise honeycomb-like structural catalystbodies, plate catalyst bodies or corrugated catalyst bodies.

In another aspect, a catalyst module is described herein comprising aframework and a plurality of structural catalyst bodies disposed in theframework, the structural catalyst bodies comprising a gradient of afirst catalytic material along the width of a surface of at least oneinner partition wall as described herein. In some embodiments, thecatalytic activity of the catalyst bodies of the module is substantiallyuniform. In being substantially uniform, catalytic activity betweencatalyst bodies of the module, in some embodiments, varies less thanabout 20%. In some embodiments, in being substantially uniform,catalytic activity between catalyst bodies of the module varies lessthan 10%. In some embodiments, in being substantially uniform, catalyticactivity between catalyst bodies of the module varies less than 5%. Insome embodiments, catalytic activity comprises the selective catalyticreduction of nitrogen oxides, the oxidation of mercury or the oxidationof ammonia or combinations thereof.

In some embodiments, sulfur dioxide oxidation activity of catalystbodies of the module is substantially uniform. In being substantiallyuniform, sulfur dioxide oxidation activity between catalyst bodies ofthe module, in some embodiments, varies less than 40%. In someembodiments, in being substantially uniform, sulfur dioxide oxidationactivity between catalyst bodies of the module varies less than 20%. Insome embodiments, in being substantially uniform, sulfur dioxideoxidation activity between catalyst bodies of the module varies lessthan 10%.

Moreover, in some embodiments, catalyst bodies of a module comprise oneor more catalytic gradients described herein in addition to a gradientof a first catalytic material along the width of a surface of at leastone inner partition wall. In some embodiments, for example, catalystbodies of the module also comprise a gradient of bulk first catalyticmaterial along a width and/or length of at least one inner partition asdescribed herein. In some embodiments, catalyst bodies of a modulecomprise one or more gradients of a second catalytic material describedherein.

In another aspect, at least one catalyst layer of a catalytic reactor isdescribed herein, the catalyst layer comprising a plurality ofstructural catalyst bodies, the structural catalyst bodies comprising agradient of catalytic material along a width of a surface of at leastone inner partition wall as described herein. In some embodiments, thecatalytic activity of the structural catalyst bodies of the catalystlayer is substantially uniform. In being substantially uniform, in someembodiments, catalytic activity between catalyst bodies of the catalystlayer varies less than about 20%. In some embodiments, in beingsubstantially uniform, catalytic activity between catalyst bodies of thecatalyst layer varies less than about 10%. In some embodiments, in beingsubstantially uniform, catalytic activity between catalyst bodies of thecatalyst layer varies less than about 5%. In some embodiments, catalyticactivity comprises the selective catalytic reduction of nitrogen oxides,the oxidation of mercury or the oxidation of ammonia or combinationsthereof.

In some embodiments, sulfur dioxide oxidation activity of catalystbodies of the catalyst layer is substantially uniform. In beingsubstantially uniform, sulfur dioxide oxidation activity betweencatalyst bodies of the catalyst layer, in some embodiments, varies lessthan 40%. In some embodiments, in being substantially uniform, sulfurdioxide oxidation activity between catalyst bodies of the catalyst layervaries less than 20%. In some embodiments, in being substantiallyuniform, sulfur dioxide oxidation activity between catalyst bodies ofthe catalyst layer varies less than 10%.

In some embodiments, catalyst bodies of a catalyst layer comprise one ormore catalytic gradients described herein in addition to the gradient ofa first catalytic material along the width of a surface of at least oneinner partition wall. In some embodiments, for example, catalyst bodiesof a catalyst layer also comprise a gradient of bulk first catalyticmaterial along a width and/or length of at least one inner partition asdescribed herein. In some embodiments, catalyst bodies of a catalystlayer comprise one or more gradients of a second catalytic materialdescribed herein. In some embodiments, catalyst bodies of a catalystlayer are arranged into one or more modules.

In another aspect, methods of treating a fluid stream, such as a fluegas or combustion gas stream, are described herein. In some embodiments,a method of treating a fluid stream comprises providing a structuralcatalyst body comprising at least one inner partition wall comprising afirst surface and a second surface opposite the first surface, the innerpartition wall having a gradient of a first catalytic material along awidth of the first surface, passing the fluid stream through thestructural catalyst body and catalytically reacting at least onechemical species in the fluid stream. In some embodiments, the fluidstream is flowed through one or more flow channels of the structuralcatalyst body. In some embodiments of methods described herein, thestructural catalyst body can have any gradient of a first catalyticmaterial and/or a second catalytic material described herein.

In some embodiments, catalytically reacting at least one chemicalspecies in the fluid stream comprises catalytically reducing nitrogenoxides in the fluid stream. In some embodiments, catalytically reactingat least one chemical species in the fluid stream comprises oxidizingammonia and/or mercury in the fluid stream.

In some embodiments of methods of treating a fluid stream, oxidation ofsulfur dioxide to sulfur trioxide in the fluid stream is reduced. In oneembodiment, for example, oxidation of sulfur dioxide is reduced duringthe selective catalytic reduction of nitrogen oxides in a fluid streamby a structural catalyst body described herein.

In some embodiments, the catalyst body is part of a module comprising aplurality of catalyst bodies described herein, where the fluid stream ispassed into the module and through the catalyst bodies. In someembodiments, the module is part of a catalytic layer of a catalyticreactor.

In another aspect, methods of producing structural catalyst bodiesdescribed herein are provided. In some embodiments, a method ofproducing a structural catalyst body comprises providing a catalystsupport comprising at least one inner partition wall comprising a firstsurface and a second surface opposite the first surface, impregnatingthe at least one inner partition wall with a solution comprising a firstcatalytic material and drying the at least one inner partition wall in amanner to establish a gradient of the first catalytic material along awidth of the first surface. In some embodiments, the first catalyticmaterial of the gradient decreases in amount at the periphery of thewidth of the first surface. In some embodiments, the first catalyticmaterial of the gradient increases in amount along a central region ofthe width of the first surface.

In some embodiments, a gradient of the first catalytic material is alsoestablished along a width of the second surface. In some embodiments,the first catalytic material of the gradient decreases in amount at theperiphery of the width of the second surface. The first catalyticmaterial of the gradient, in some embodiments, increases in amount alonga central region of the width of the second surface. In someembodiments, the gradient profile of the first catalytic material alongthe width of the second surface is symmetrical or substantiallysymmetrical to the gradient profile of the first catalytic materialalong the width of the first surface.

In some embodiments, the at least one inner partition wall of thestructural catalyst support is dried in a manner to establish a gradientof bulk first catalytic material along a width of the inner partitionwall. In some embodiments, bulk first catalytic material of the gradientdecreases in concentration at the periphery of the width of the innerpartition wall. In some embodiments, bulk first catalytic materialincreases in concentration along a central region of the width of theinner partition wall. In some embodiments, a gradient of a bulk firstcatalytic material along the width of the inner partition wall has aprofile symmetrical or substantially symmetrical about the midpoint ofthe profile.

In some embodiments, the at least one inner partition wall of thestructural catalyst support is dried in a manner to establish a gradientof the first catalyst material along a length of the first surface ofthe inner partition wall. A gradient of the first catalytic materialalong the length of a first surface of the inner partition wall, in someembodiments, comprises a greater amount of the first catalytic materialat a first end of the inner partition wall in comparison with an amountof the first catalytic material at a second end of the inner partitionwall, the second end opposite the first end.

In some embodiments, a gradient of the first catalytic material is alsoestablished along a length of the second surface of the inner partitionwall. A gradient of the first catalytic material along the length of thesecond surface of the inner partition wall, in some embodiments,comprises a greater amount of the first catalytic material at a firstend of the inner partition wall in comparison with an amount of thefirst catalytic material at a second end of the inner partition wall,the second end opposite the first end. In some embodiments, the gradientprofile of the first catalytic material along the length of the secondsurface of the inner partition wall is symmetrical or substantiallysymmetrical to the gradient profile of the first catalytic materialalong the length of the first surface of the inner partition wall.

In some embodiments, the first end of the inner partition wallcorresponds to the fluid stream inlet side of the structural catalystbody and the second end corresponds to the fluid stream outlet side ofthe structural catalyst body. Alternatively, in some embodiments, thefirst end of the inner partition wall corresponds to the outlet side ofthe structural catalyst body, and the second end corresponds to thefluid stream inlet side.

In some embodiments, the at least one inner partition wall of astructural catalyst body described herein is dried in a manner toestablish a gradient of a bulk first catalytic material along a lengthof the inner partition wall. In some embodiments, a gradient of a firstbulk catalytic material along a length of the inner partition wallcomprises a greater concentration of the bulk first catalytic materialat a first end of the inner partition wall in comparison with aconcentration of the bulk first catalytic material at a second end ofthe inner partition wall, the second end opposite the first end.

In some embodiments of methods described herein, the structural catalystbody comprises a plurality of inner partition walls such that the innerpartition walls are impregnated with a solution comprising the firstcatalytic material and dried in a manner to establish a gradient of theof the first catalytic material along a width and/or length of one ormore surfaces of the inner partition walls. In some embodiments, theinner partition walls are dried in a manner to establish a gradient of abulk first catalytic material along a width and/or length of the innerpartition walls.

In some embodiments, inner partition walls of a structural catalyst bodyproduced according to methods described herein intersect to form one ormore centerposts. In some embodiments, at least one centerpost isimpregnated with a solution comprising the first catalytic material anddried in a manner to establish a gradient of bulk first catalyticmaterial between the centerpost and at least one of the inner partitionwalls. In some embodiments, for example, at least one inner partitionwall comprises a greater concentration of bulk first catalytic materialthan the centerpost. In some embodiments, each of the inner partitionwalls connected to the centerpost comprises a greater concentration ofbulk first catalytic material than the centerpost.

In some embodiments of methods described herein, the impregnatingsolution further comprises a second catalytic material. In someembodiments, a gradient of bulk metal or metal oxide second catalyticmaterial is established along a width of the inner partition wall.Alternatively, in some embodiments, at least one inner partition wall ofa structural catalyst body comprising one or more gradients of the firstcatalytic material described herein is further impregnated with asolution comprising a metal or metal oxide second catalytic material anddried in a manner to establish a gradient of the metal or metal oxidesecond catalytic material along a width of the first surface and/orsecond surface of the inner partition wall. In some embodiments, agradient of bulk metal or metal oxide second catalytic material isestablished along a width of the inner partition wall.

In some embodiments, the second catalytic material of the gradientdecreases in amount at the periphery of the width of the first surface.In some embodiments, the second catalytic material of the gradientincreases in amount along a central region of the width of the firstsurface.

In some embodiments, a gradient of the second catalytic material is alsoestablished along a width of the second surface of the inner partitionwall. In some embodiments, the second catalytic material of the gradientdecreases in amount at the periphery of the width of the second surface.The second catalytic material of the gradient, in some embodiments,increases in amount along a central region of the width of the secondsurface. In some embodiments, the gradient profile of the secondcatalytic material along the width of the second surface is symmetricalor substantially symmetrical to the gradient profile of the secondcatalytic material along the width of the first surface.

In some embodiments, a gradient of the second catalytic material is alsoestablished along a length of the first surface of the inner partitionwall. A gradient of the second catalytic material along a first surfaceof the inner partition wall, in some embodiments, comprises a greateramount of the second catalytic material at a first end of the innerpartition wall in comparison with an amount of the second catalyticmaterial at a second end of the inner partition wall, the second endopposite the first end.

In some embodiments, a gradient of the second catalytic material is alsoestablished along a length of the second surface of the inner partitionwall. A gradient of the second catalytic material along the length ofthe second surface of the inner partition wall, in some embodiments,comprises a greater amount of the second catalytic material at a firstend of the inner partition wall in comparison with an amount of thesecond catalytic material at a second end of the inner partition wall,the second end opposite the first end. In some embodiments, the gradientprofile of the second catalytic material along the length of the secondsurface of the inner partition wall is symmetrical or substantiallysymmetrical to the gradient profile of the second catalytic materialalong the length of the first surface of the inner partition wall.

In some embodiments, a gradient of bulk second catalytic material isalso established along a width of the inner partition wall. In someembodiments, bulk second catalytic material of the gradient decreases inconcentration at the periphery of the width of the inner partition wall.In some embodiments, bulk second catalytic material increases inconcentration along a central region of the width of the inner partitionwall. In some embodiments, a gradient of bulk second catalytic materialalong the width of the inner partition wall has a profile symmetrical orsubstantially symmetrical about the midpoint of the profile.

In some embodiments, drying the at least one inner partition wall of astructural catalyst body described herein also establishes a gradient ofa bulk second catalytic material along a length of the inner partitionwall. In some embodiments, a gradient of a bulk second catalyticmaterial along a length of the inner partition wall comprises a greaterconcentration of the bulk second catalytic material at a first end ofthe inner partition wall in comparison with a concentration of the bulksecond catalytic material at a second end of the inner partition wall,the second end opposite the first end.

Moreover, in some embodiments of methods described herein, a gradient ofthe second catalytic material is also established along a width and/orlength of one or more surfaces of a plurality of inner partition wallsof the structural catalyst body. In some embodiments, a gradient of bulksecond catalytic material is also established along a width and/orlength of a plurality of inner partition walls of the structuralcatalyst body.

In some embodiments, at least one centerpost of a structural catalystbody is impregnated with the solution further comprising the secondcatalytic material, and drying the structural catalyst body alsoestablishes a gradient of bulk second catalytic material between thecenterpost and at least one of the inner partition walls forming thecenterpost. In some embodiments, for example, at least one innerpartition wall comprises a greater concentration of bulk secondcatalytic material than the centerpost. In some embodiments, each of theinner partition walls forming the centerpost comprises a greaterconcentration of bulk second catalytic material than the centerpost.

Additionally, in some embodiments, the outer peripheral wall of astructural catalyst body described herein is impregnated with the secondcatalytic material. In some embodiments wherein the outer peripheralwall comprises bulk second catalytic material, inner partition walls ofthe structural catalyst body comprise a greater concentration of bulksecond catalytic material than the outer peripheral wall.

In some embodiments, first and/or second catalytic material of gradientsof structural catalyst bodies produced according to methods describedherein comprise one or more transition metals. In some embodiments,transition metals of the first and/or second catalytic material comprisevanadium, tungsten, molybdenum, platinum, palladium, ruthenium, rhodium,rhenium, iron, gold, silver, copper or nickel or alloys or oxidesthereof. In some embodiments, the first and/or second catalytic materialof gradients of structural catalyst bodies described herein are suitablefor SCR applications and processes. In some embodiments, for example,the first and/or second catalytic material comprise V₂O₅, WO₃ or MoO₃ ormixtures thereof. In some embodiments, the first and/or second catalyticmaterial comprise one or more precursors for forming a catalyticmaterial suitable for SCR applications. In some embodiments, forexample, the first and/or second catalytic material comprise one or moreprecursors for forming V₂O₅, WO₃ or MoO₃ or mixtures thereof.

In some embodiments, drying inner partition walls and/or centerposts ofa structural catalyst support comprises flowing a gas over surfaces ofthe inner partition walls and/or centerposts at a rate and/ortemperature sufficient to establish one or more gradients of the firstcatalytic material and/or second catalytic material described herein.Flowing a gas over surfaces of the inner partition walls and/orcenterposts to establish one or more gradients of the first catalyticmaterial and/or second catalytic material described herein can beadministered in any manner not inconsistent with the objectives of thepresent invention. In some embodiments, gas is flowed over all orsubstantially all of the inner partition walls and/or centerposts of astructural catalyst support in an even or substantially even manner.

Additionally, in some embodiments, the impregnation solution of a methoddescribed herein further comprises at least one additional catalyticmaterial. In such embodiments, drying the structural catalyst body canprovide one or more gradients of the additional catalytic materialhaving a construction and/or location on the structural catalyst bodyconsistent with any gradient of the first and/or second catalyticmaterial described herein.

In some embodiments, a structural catalyst support is virgin. A virginstructural catalyst support, in some embodiments, has not been used orpreviously installed into a catalytic reactor for conducting catalyticreactions in a fluid stream.

In some embodiments, a structural catalyst support is used. A usedstructural catalyst support, in some embodiments, has been previouslyinstalled in a catalytic reactor for conducting catalytic reactions in afluid stream. In some embodiments, a used catalyst support is part of astructural catalyst body in need of regeneration.

In some embodiments, virgin or used structural catalyst supportscomprise honeycomb-like structural supports, plate structural supportsor corrugated structural supports.

In some embodiments of methods described herein, structural catalystsupports comprising a plurality of inner partition walls are arranged inthe framework of a catalyst module. In such embodiments, the catalystmodule comprising the structural catalyst supports can be immersed inthe solution of catalytic material to impregnate the inner partitionwalls and/or centerposts of the structural catalyst supports withcatalytic material.

In some embodiments, the structural catalyst supports impregnated with asolution of the first catalytic material are dried while remaining theframework of the catalyst module to establish one or more gradients ofthe first catalytic material described herein. In some embodiments, theimpregnation solution further comprises a second catalytic materialwherein drying the structural catalyst supports while remaining in theframework of the catalyst module also establishes one or more gradientsof the second catalytic material as described herein. In someembodiments, for example, a gas is flowed through the module and oversurfaces of the inner partition walls and/or centerposts of thestructural catalyst supports at a rate and/or temperature sufficient toestablish one or more gradients of the first and/or second catalyticmaterial described herein. In some embodiments, the gas is flowed evenlyor substantially evenly through the structural catalyst supportsarranged in the framework of the module such that the catalytic activityof the resulting structural catalyst bodies is substantially uniformacross the module. In being substantially uniform, catalytic activitybetween catalyst bodies in the module, in some embodiments, varies lessthan about 20%. In some embodiments, in being substantially uniform,catalytic activity between catalyst bodies of the module varies lessthan 10%. In some embodiments, in being substantially uniform, catalyticactivity between catalyst bodies of the module varies less than 5%. Insome embodiments, catalytic activity comprises the selective catalyticreduction of nitrogen oxides, the oxidation of mercury or the oxidationof ammonia or combinations thereof.

In some embodiments, sulfur dioxide oxidation activity of catalystbodies of the module is substantially uniform across the module. Inbeing substantially uniform, sulfur dioxide oxidation activity betweencatalyst bodies of the module, in some embodiments, varies less than40%. In some embodiments, in being substantially uniform, sulfur dioxideoxidation activity between catalyst bodies of the module varies lessthan 20%. In some embodiments, in being substantially uniform, sulfurdioxide oxidation activity between catalyst bodies of the module variesless than 10%.

In some embodiments, gradients of first and/or second catalytic materialproduced according to the forgoing methods can have any of thestructural and/or compositional properties described herein for thegradients of the first and/or second catalytic material.

These and other embodiments are described in greater detail in thedetailed description which follows.

BRIEF DESCRIPTION OF THE DRAWINGS

FIG. 1 illustrates gradient profiles of first and second catalyticmaterials along the width of the surface of an inner partition wall of astructural catalyst body according to one embodiment described herein.

FIG. 2 illustrates a structural catalyst body according to oneembodiment described herein.

FIG. 3 illustrates a cross-section of a portion of a structural catalystbody according to one embodiment described herein.

FIG. 4 illustrates catalytic activity testing of a structural catalystbody according to one embodiment described herein in comparison to aprior structural catalyst body.

FIG. 5 provides a table detailing structural catalyst bodies havingvarious gradient composition according to some embodiments describedherein.

FIG. 6 illustrates a cross-section of a portion of a corrugatedstructural catalyst body according to one embodiment described herein.

DETAILED DESCRIPTION

The present invention can be understood more readily by reference to thefollowing detailed description, examples and drawings and their previousand following descriptions. Elements, apparatus and methods of thepresent invention, however, are not limited to the specific embodimentspresented in the detailed description, examples and drawings. It shouldbe recognized that these embodiments are merely illustrative of theprinciples of the present invention. Numerous modifications andadaptations will be readily apparent to those of skill in the artwithout departing from the spirit and scope of the invention.

Moreover, all ranges disclosed herein are to be understood to encompassany and all subranges subsumed therein. For example, a stated range of“1 to 10” should be considered to include any and all subranges between(and inclusive of) the minimum value of 1 and the maximum value of 10;that is, all subranges beginning with a minimum value of 1 or more, e.g.1 to 6.1, and ending with a maximum value of 10 or less, e.g., 5.5 to10. Additionally, any reference referred to as being “incorporatedherein” is to be understood as being incorporated in its entirety.

It is further noted that, as used in this specification, the singularforms “a,” “an,” and “the” include plural referents unless expressly andunequivocally limited to one referent.

In one aspect, catalyst bodies are described herein which, in someembodiments, display heterogeneous distributions of catalytic material.In some embodiments, catalyst bodies described herein are operable forthe selective catalytic reduction of nitrogen oxides in a flue gasstream.

In some embodiments, a structural catalyst body described hereincomprises at least one inner partition wall comprising a first surfaceand a second surface opposite the first surface, the inner partitionwall having a gradient of a first catalytic material along a width ofthe first surface. In some embodiments, the first catalytic material ofthe gradient decreases in amount at the periphery of the width of thefirst surface.

In some embodiments, the surface of an inner partition wall of astructural catalyst body described herein includes a portion of theinner partition wall up to a depth of about 100 μm. In some embodiments,the surface of an inner partition wall includes a portion of the innerpartition wall up to a depth of about 50 μm or up to about 25 μm. Insome embodiments, the surface of an inner partition wall includes aportion of the inner partition wall up to a depth of about 10 μm or upto about 5 μm.

In some embodiments, the first catalytic material of the gradientincreases in amount along a central region of the width of the firstsurface. In some embodiments, the amount of the first catalytic materialin a central region of the width of the first surface exceeds the amountof the first catalytic material at the periphery of the width of thefirst surface. In some embodiments, the amount of the first catalyticmaterial at a point in a central region of the width of the firstsurface is greater than the amount of the first catalytic material at apoint at the periphery of the width of the first surface.

In some embodiments, the amount of the first catalytic material at apoint in a central region of the width of the first surface is at least1.1 times greater or 1.3 times greater than the amount of the firstcatalytic material at a point at the periphery of the width of the firstsurface. In some embodiments, the amount of the first catalytic materialat a point in a central region of the width of the first surface is atleast 1.5 times or at least 2 times greater than the amount of the firstcatalytic material at a point at the periphery of the width of the firstsurface. In some embodiments, the amount of the first catalytic materialat a point in a central region of the width of the first surface is atleast 3 times or at least 3.5 times greater than the amount of the firstcatalytic material at a point at the periphery of the width of the firstsurface. In some embodiments, the amount of the first catalytic materialat a point in a central region of the width of the first surface is atleast 4 times or at least 4.5 times greater than the amount of the firstcatalytic material at a point at the periphery of the width of the firstsurface. In some embodiments, the amount of the first catalytic materialat a point in a central region of the width of the first surface is atleast 5 times or at least 10 times greater than the amount of the firstcatalytic material at a point at the periphery of the width of the firstsurface. In some embodiments, an amount of the first catalytic materialat a plurality of points in a central region of the width of the firstsurface is at least 1.1 times greater or 1.3 times greater than anamount of the first catalytic material at one or more points at theperiphery of the width of the first surface.

In some embodiments, the amount of the first catalytic material at pointin a central region of the width of the first surface is 1.3 times to 10times greater than the amount of the first catalytic material at a pointat the periphery of the width of the first surface. In some embodiments,the amount of the first catalytic material at a plurality of points in acentral region of the width of the first surface is 1.3 times to 10times greater than the amount of the first catalytic material at one ormore points at the periphery of the width of the first surface.

In some embodiments of a section of an inner partition wall, the averageamount of the first catalytic material in a central region of the widthof the first surface of the inner partition wall section is at least 1.5times greater than the average amount of the first catalytic material atthe periphery of the width of the first surface of the inner partitionwall section.

In some embodiments, a central region of the width of the first surfacecomprises up to about 20 percent of the total width of the firstsurface, the central region centered around the midpoint of the width ofthe first surface. In some embodiments, a central region of the width ofthe first surface comprises up to about 40 percent of the total width ofthe first surface, the central region centered around the midpoint ofthe width of the first surface.

In some embodiments, the periphery of the width of the first surfacecomprises up to about 15 percent of the total width of the first surfacebeginning at the edge of the width of the first surface and extending ina direction toward the central region.

In some embodiments, a gradient of a first catalytic material along thewidth of the first surface of the inner partition wall has a profilesymmetrical or substantially symmetrical about the midpoint of theprofile.

A structural catalyst body described herein, in some embodiments,further comprises a gradient of the first catalytic material along awidth of the second surface. In some embodiments, the first catalyticmaterial of the gradient decreases in amount at the periphery of thewidth of the second surface. The first catalytic material of thegradient, in some embodiments, increases in amount along a centralregion of the second surface.

In some embodiments, the amount of the first catalytic material at apoint in a central region of the width of the second surface is at least1.1 times greater or 1.3 times greater than the amount of the firstcatalytic material at a point at the periphery of the width of thesecond surface. In some embodiments, the amount of the first catalyticmaterial at a point in a central region of the width of the secondsurface is at least 1.5 times or at least 2 times greater than theamount of the first catalytic material at a point at the periphery ofthe width of the second surface. In some embodiments, the amount of thefirst catalytic material at a point in a central region of the width ofthe second surface is at least 3 times or at least 3.5 times greaterthan the amount of the first catalytic material at a point at theperiphery of the width of the second surface. In some embodiments, theamount of the first catalytic material at a point in a central region ofthe width of the second surface is at least 4 times or at least 4.5times greater than the amount of the first catalytic material at a pointat the periphery of the width of the second surface. In someembodiments, the amount of the first catalytic material at a point in acentral region of the width of the second surface is at least 5 times orat least 10 times greater than the amount of the first catalyticmaterial at a point at the periphery of the width of the second surface.In some embodiments, an amount of the first catalytic material at aplurality of points in a central region of the width of the secondsurface is at least 1.1 times greater or 1.3 times greater than theamount of the first catalytic material at one or more points at theperiphery of the width of the second surface.

In some embodiments, the amount of the first catalytic material at apoint in a central region of the width of the second surface is 1.3times to 10 times greater than the amount of the first catalyticmaterial at a point at the periphery of the width of the second surface.In some embodiments, the amount of the first catalytic material at aplurality of points in a central region of the width of the secondsurface is 1.3 times to 10 times greater than the amount of the firstcatalytic material at one or more points at the periphery of the widthof the second surface.

In some embodiments of a section of an inner partition wall, the averageamount of the first catalytic material in a central region of the widthof the second surface of the inner partition wall section is at least1.5 times greater than the average amount of the first catalyticmaterial at the periphery of the width of the second surface of theinner partition wall section.

In some embodiments, a central region of the width of the second surfacecomprises up to about 20 percent of the total width of the secondsurface, the central region centered around the midpoint of the width ofthe second surface. In some embodiments, a central region of the widthof the second surface comprises up to about 40 percent of the totalwidth of the second surface, the central region centered around themidpoint of the width of the second surface.

In some embodiments, a periphery of the width of the second surfacecomprises up to about 15 percent of the total width of the secondsurface beginning at the edge of the width of the second surface andextending in a direction toward the central region.

In some embodiments, a gradient of the first catalytic material alongthe width of the second surface of the inner partition wall has aprofile symmetrical or substantially symmetrical about the midpoint ofthe profile.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of a second catalytic material along the width ofthe first surface of the at least one inner partition wall. In someembodiments, the second catalytic material of the gradient decreases inamount at the periphery of the width of the first surface.

In some embodiments, the second catalytic material of the gradientincreases in amount along a central region of the width of the firstsurface. In some embodiments, the amount of the second catalyticmaterial in a central region of the width of the first surface exceedsthe amount of the second catalytic material at the periphery of thewidth of the first surface. In some embodiments, the amount of thesecond catalytic material at a point in a central region of the width ofthe first surface is greater than the amount of the second catalyticmaterial at a point at the periphery of the width of the first surface.

In some embodiments, the amount of the second catalytic material at apoint in a central region of the width of the first surface is at least1.1 times greater or 1.3 times greater than the amount of the secondcatalytic material at a point at the periphery of the width of the firstsurface. In some embodiments, the amount of the second catalyticmaterial at a point in a central region of the width of the firstsurface is at least 1.5 times or at least 2 times greater than theamount of the second catalytic material at a point at the periphery ofthe width of the first surface. In some embodiments, the amount of thesecond catalytic material at a point in a central region of the width ofthe first surface is at least 3 times or at least 3.5 times greater thanthe amount of the second catalytic material at a point at the peripheryof the width of the first surface. In some embodiments, the amount ofthe second catalytic material at a point in a central region of thewidth of the first surface is at least 4 times or at least 4.5 timesgreater than the amount of the second catalytic material at a point atthe periphery of the width of the first surface. In some embodiments,the amount of the second catalytic material at a point in a centralregion of the width of the first surface is at least 5 times or at least10 times greater than the amount of the second catalytic material at apoint at the periphery of the width of the first surface. In someembodiments, an amount of the second catalytic material at a pluralityof points in a central region of the width of the first surface is atleast 1.1 times greater or 1.3 times greater than an amount of thesecond catalytic material at one or more points at the periphery of thewidth of the first surface.

In some embodiments, the amount of the second catalytic material atpoint in a central region of the width of the first surface is 1.3 timesto 10 times greater than the amount of the second catalytic material ata point at the periphery of the width of the first surface. In someembodiments, the amount of the second catalytic material at a pluralityof points in a central region of the width of the first surface is 1.3times to 10 times greater than the amount of the second catalyticmaterial at one or more points at the periphery of the width of thefirst surface.

In some embodiments, a gradient of a second catalytic material along thewidth of the first surface of the inner partition wall has a profilesymmetrical or substantially symmetrical about the midpoint of theprofile.

In some embodiments of a section of an inner partition wall, the averageamount of the second catalytic material in a central region of the widthof the first surface of the inner partition wall section is at least 1.5times greater than the average amount of the second catalytic materialat the periphery of the width of the first surface of the innerpartition wall section.

A structural catalyst body described herein, in some embodiments,further comprises a gradient of the second catalytic material along awidth of the second surface. In some embodiments, the second catalyticmaterial of the gradient decreases in amount at the periphery of thewidth of the second surface. The second catalytic material of thegradient, in some embodiments, increases in amount along a centralregion of the second surface.

In some embodiments, the amount of the second catalytic material at apoint in a central region of the width of the second surface is at least1.1 times greater or 1.3 times greater than the amount of the secondcatalytic material at a point at the periphery of the width of thesecond surface. In some embodiments, the amount of the second catalyticmaterial at a point in a central region of the width of the secondsurface is at least 1.5 times or at least 2 times greater than theamount of the second catalytic material at a point at the periphery ofthe width of the second surface. In some embodiments, the amount of thesecond catalytic material at a point in a central region of the width ofthe second surface is at least 3 times or at least 3.5 times greaterthan the amount of the second catalytic material at a point at theperiphery of the width of the second surface. In some embodiments, theamount of the second catalytic material at a point in a central regionof the width of the second surface is at least 4 times or at least 4.5times greater than the amount of the second catalytic material at apoint at the periphery of the width of the second surface. In someembodiments, the amount of the second catalytic material at a point in acentral region of the width of the second surface is at least 5 times orat least 10 times greater than the amount of the second catalyticmaterial at a point at the periphery of the width of the second surface.In some embodiments, the amount of the second catalytic material at aplurality of points in a central region of the width of the secondsurface is at least 1.1 times greater or 1.3 times greater than theamount of the second catalytic material at one or more points at theperiphery of the width of the second surface.

In some embodiments, the amount of the second catalytic material at apoint in a central region of the width of the second surface is 1.3times to 10 times greater than the amount of the second catalyticmaterial at a point at the periphery of the width of the second surface.In some embodiments, the amount of the second catalytic material at aplurality of points in a central region of the width of the secondsurface is 1.3 times to 10 times greater than the amount of the secondcatalytic material at one or more points at the periphery of the widthof the second surface.

In some embodiments of a section of an inner partition wall, the averageamount of the second catalytic material in a central region of the widthof the second surface of the inner partition wall section is at least1.5 times greater than the average amount of the second catalyticmaterial at the periphery of the width of the second surface of theinner partition wall section.

In some embodiments, a gradient of the first catalytic material alongthe width of the second surface of the inner partition wall has aprofile symmetrical or substantially symmetrical about the midpoint ofthe profile.

FIG. 1 illustrates gradient profiles of first and second catalyticmaterials along the width of the surface of an inner partition wall of astructural catalyst body according to one embodiment described herein.As illustrated in FIG. 1, the first catalytic material of vanadiumpentoxide (V₂O₅) and the second catalytic material of tungsten oxide(WO₃) increase in amount along a central region of the width of theinner partition wall surface. Moreover, the V₂O₅ first catalyticmaterial and the WO₃ second catalytic material decrease in amount at theperiphery of the width of the inner partition wall surface. The profilesof the V₂O₅ first catalytic material and the WO₃ second catalyticmaterial are also substantially symmetrical about the midpoints of theprofiles.

In some embodiments, a structural catalyst body described hereincomprises a gradient of bulk first catalytic material along the width ofat least one inner partition wall. In some embodiments, bulk firstcatalytic material of the gradient decreases in concentration at theperiphery of the width of the inner partition wall. In some embodiments,bulk first catalytic material increases in concentration along a centralregion of the width of the inner partition wall. In some embodiments, agradient of bulk first catalytic material along the width of the innerpartition wall has a profile symmetrical or substantially symmetricalabout the midpoint of the profile.

In some embodiments, the concentration of bulk first catalytic materialat a point in a central region of the width of the inner partition wallis at least 1.1 times greater or 1.3 times greater than theconcentration of bulk first catalytic material at a point at theperiphery of the width of the inner partition wall. In some embodiments,the concentration of bulk first catalytic material at a point in acentral region of the width of the inner partition wall is at least 1.5times or at least 2 times greater than the concentration of bulk firstcatalytic material at a point at the periphery of the width of the innerpartition wall. In some embodiments, the concentration of bulk firstcatalytic material at a point in a central region of the width of theinner partition wall is at least 3 times or at least 3.5 times greaterthan the concentration of bulk first catalytic material at a point atthe periphery of the width of the inner partition wall. In someembodiments, the concentration of bulk first catalytic material at apoint in a central region of the width of the inner partition wall is atleast 4 times or at least 4.5 times greater than the concentration ofbulk first catalytic material at a point at the periphery of the widthof the inner partition wall. In some embodiments, the concentration ofbulk first catalytic material at a point in a central region of thewidth of the inner partition wall is at least 5 times or at least 10times greater than the concentration of bulk first catalytic material ata point at the periphery of the width of the inner partition wall. Insome embodiments, the concentration of bulk first catalytic material ata plurality of points in a central region of the width of the innerpartition wall is at least 1.1 times greater or 1.3 times greater thanthe concentration of bulk first catalytic material at one or more pointsat the periphery of the width of the inner partition wall.

In some embodiments, the concentration of bulk first catalytic materialat a point in a central region of the width of the inner partition wallis 1.3 times to 10 times greater than the concentration of bulk firstcatalytic material at a point at the periphery of the width of the innerpartition wall. In some embodiments, a concentration of bulk firstcatalytic material at a plurality of points in the central region of thewidth of the inner partition wall is 1.3 times to 10 times greater thanthe concentration of bulk first catalytic material at one or more pointsat the periphery of the width of the inner partition wall.

In some embodiments, a central region of the width of the innerpartition wall comprises up to about 20 percent of the total width ofthe inner partition wall, the central region centered around themidpoint of the width of the inner partition wall. In some embodiments,a central region of the width of the inner partition wall comprises upto about 40 percent of the total width of the inner partition wall, thecentral region centered around the midpoint of the width of the innerpartition wall.

In some embodiments, a periphery of the width of the inner partitionwall comprises up to about 15 percent of the total width of the innerpartition wall beginning at the edge of the width of the inner partitionwall and extending in a direction toward the central region.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of bulk second catalytic material along the widthof the at least one inner partition wall comprising the gradient of bulkfirst catalytic material.

In some embodiments, bulk second catalytic material of the gradientdecreases in concentration at the periphery of the width of the innerpartition wall. In some embodiments, bulk second catalytic materialincreases in concentration along a central region of the width of theinner partition wall. In some embodiments, a gradient of bulk secondcatalytic material along the width of the inner partition wall has aprofile symmetrical or substantially symmetrical about the midpoint ofthe profile.

In some embodiments, the concentration of bulk second catalytic materialat a point in a central region of the width of the inner partition wallis at least 1.1 times greater or 1.3 times greater than theconcentration of bulk second catalytic material at a point at theperiphery of the width of the inner partition wall. In some embodiments,the concentration of bulk second catalytic material at a point in acentral region of the width of the inner partition wall is at least 1.5times or at least 2 times greater than the concentration of bulk secondcatalytic material at a point at the periphery of the width of the innerpartition wall. In some embodiments, the concentration of bulk secondcatalytic material at a point in a central region of the width of theinner partition wall is at least 3 times or at least 3.5 times greaterthan the concentration of bulk second catalytic material at a point atthe periphery of the width of the inner partition wall. In someembodiments, the concentration of bulk second catalytic material at apoint in a central region of the width of the inner partition wall is atleast 4 times or at least 4.5 times greater than the concentration ofbulk second catalytic material at a point at the periphery of the widthof the inner partition wall. In some embodiments, the concentration ofbulk second catalytic material at a point in a central region of thewidth of the inner partition wall is at least 5 times or at least 10times greater than the concentration of bulk second catalytic materialat a point at the periphery of the width of the inner partition wall. Insome embodiments, the concentration of bulk second catalytic material ata plurality of points in a central region of the width of the innerpartition wall is at least 1.1 times greater or 1.3 times greater thanthe concentration of bulk second catalytic material at one or morepoints at the periphery of the width of the inner partition wall.

In some embodiments, the concentration of bulk second catalytic materialat a point in a central region of the width of the inner partition wallis 1.3 times to 10 times greater than the concentration of bulk secondcatalytic material at a point at the periphery of the width of the innerpartition wall. In some embodiments, the concentration of bulk secondcatalytic material at a plurality of points in the central region of thewidth of the inner partition wall is 1.3 times to 10 times greater thanthe concentration of bulk second catalytic material at one or morepoints at the periphery of the width of the inner partition wall.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of first catalytic material along a length of thefirst surface of the inner partition wall. A gradient of first catalyticmaterial along the length of the first surface of the inner partitionwall, in some embodiments, comprises a greater amount of first catalyticmaterial at a first end of the inner partition wall in comparison withan amount of the first catalytic material at a second end of the innerpartition wall, the second end opposite the first end. In someembodiments, the amount of first catalytic material at a point on thefirst surface at the first end of the inner partition wall is 1.3 timesto 10 times greater than the amount of the first catalytic material at apoint on the first surface at the second end of the inner partitionwall. In some embodiments, the amount of first catalytic material at apoint on the first surface at the first end of the inner partition wallis at least 10 times greater than the amount of first catalytic materialat a point on the first surface at the second end of the inner partitionwall.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of second catalytic material along a length of thefirst surface of the inner partition wall. A gradient of secondcatalytic material along the length of the first surface of the innerpartition wall, in some embodiments, comprises a greater amount ofsecond catalytic material at a first end of the inner partition wall incomparison with an amount of the second catalytic material at a secondend of the inner partition wall, the second end opposite the first end.In some embodiments, the amount of second catalytic material at a pointon the first surface at the first end of the inner partition wall is 1.3times to 10 times greater than the amount of the second catalyticmaterial at a point on the first surface at the second end of the innerpartition wall. In some embodiments, the amount of second catalyticmaterial at a point on the first surface at the first end of the innerpartition wall is at least 10 times greater than the amount of secondcatalytic material at a point on the first surface at the second end ofthe inner partition wall.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of first catalytic material along a length of thesecond surface of the inner partition wall. A gradient of firstcatalytic material along the length of the second surface of the innerpartition wall, in some embodiments, comprises a greater amount of thefirst catalytic material at a first end of the inner partition wall incomparison with an amount of the first catalytic material at a secondend of the inner partition wall, the second end opposite the first end.In some embodiments, the amount of the first catalytic material at apoint on the second surface at the first end of the inner partition wallis 1.3 times to 10 times greater than the amount of the first catalyticmaterial at a point on the second surface at the second end of the innerpartition wall. In some embodiments, the amount of the first catalyticmaterial at a point on the second surface at the second end of the innerpartition wall is at least 10 times greater than the amount of the firstcatalytic material at a point on the second surface at the second end ofthe inner partition wall.

In some embodiments, the gradient of the first catalytic material alongthe length of the second surface of the inner partition wall issymmetrical or substantially symmetrical to the gradient of the firstcatalytic material along the length of the first surface of the innerpartition wall.

In some embodiments, the first end of the inner partition wallcorresponds to the fluid stream inlet side of the structural catalystbody and the second end corresponds to the fluid stream outlet side ofthe structural catalyst body.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of second catalytic material along a length of thesecond surface of the inner partition wall. A gradient of secondcatalytic material along the length of the second surface of the innerpartition wall, in some embodiments, comprises a greater amount of thesecond catalytic material at a first end of the inner partition wall incomparison with an amount of the second catalytic material at a secondend of the inner partition wall, the second end opposite the first end.In some embodiments, the amount of the second catalytic material at apoint on the second surface at the first end of the inner partition wallis 1.3 times to 10 times greater than the amount of the second catalyticmaterial at a point on the second surface at the second end of the innerpartition wall. In some embodiments, the amount of the second catalyticmaterial at a point on the second surface at the second end of the innerpartition wall is at least 10 times greater than the amount of thesecond catalytic material at a point on the second surface at the secondend of the inner partition wall.

In some embodiments, the gradient of the second catalytic material alongthe length of the second surface of the inner partition wall issymmetrical or substantially symmetrical to the gradient of the secondcatalytic material along the length of the first surface of the innerpartition wall.

In some embodiments, a structural catalyst body described hereincomprises a gradient of bulk first catalytic material along a length ofat least one inner partition wall. In some embodiments, a gradient ofbulk first catalytic material along a length of the inner partition wallcomprises a greater concentration of bulk first catalytic material at afirst end of the inner partition wall in comparison with a concentrationof bulk first catalytic material at a second end of the inner partitionwall, the second end opposite the first end. As described herein, insome embodiments, the first end of the inner partition wall correspondsto the fluid stream inlet side of the structural catalyst body and thesecond end corresponds to the fluid stream outlet side of the structuralcatalyst body.

In some embodiments, the concentration of bulk first catalytic materialat a point at the first end of the inner partition wall is 1.3 times to10 times greater than the concentration of bulk first catalytic materialat a point at the second end of the inner partition wall. In someembodiments, the concentration of bulk first catalytic material at apoint at the first end of the inner partition wall is at least 10 timesgreater than the concentration of bulk first catalytic material at apoint at the second end of the inner partition wall.

In some embodiments, a structural catalyst body described herein furthercomprises a gradient of bulk second first catalytic material along alength of at least one inner partition wall. In some embodiments, agradient of a bulk second catalytic material along a length of the innerpartition wall comprises a greater concentration of bulk secondcatalytic material at a first end of the inner partition wall incomparison with a concentration of bulk second catalytic material at asecond end of the inner partition wall, the second end opposite thefirst end.

In some embodiments, the concentration of bulk second catalytic materialat a point at the first end of the inner partition wall is 1.3 times to10 times greater than the concentration of bulk second catalyticmaterial at a point at the second end of the inner partition wall. Insome embodiments, the concentration of bulk second catalytic material ata point at the first end of the inner partition wall is at least 10times greater than the concentration of bulk second catalytic materialat a point at the second end of the inner partition wall.

A structural catalyst body described herein, in some embodiments,further comprises at least one additional inner partition wallcomprising one or more gradients of first catalytic material and/orsecond catalytic material described herein for an inner partition wall.In some embodiments, the at least one additional inner partition wallcomprises a first surface and a second surface and a gradient of firstcatalytic material and/or second catalytic material along a width of thefirst surface. In some embodiments, the at least one additional innerpartition wall further comprises a gradient of first catalytic materialand/or second catalytic material along a width of the second surface. Agradient of first catalytic material and/or second catalytic materialalong the width of the first surface and/or the second surface of the atleast one additional inner partition wall, in some embodiments, has oneor more properties consistent with the same described for the innerpartition wall hereinabove.

Moreover, in some embodiments, the at least one additional innerpartition wall comprises a gradient of bulk first catalytic materialand/or bulk second catalytic material along a width of the additionalinner partition wall. In some embodiments, the at least one additionalinner partition wall comprises a gradient of bulk first catalyticmaterial and/or second catalytic material along a length of the innerpartition wall.

The at least one additional inner partition wall, in some embodiments,comprises a gradient of first catalytic material and/or second catalyticmaterial along the length of the first surface and/or second surface. Agradient of the first catalytic material and/or second catalyticmaterial along the length of the first surface and/or the second surfaceof the at least one additional inner partition wall, in someembodiments, has one or more properties consistent with the samedescribed for the inner partition wall hereinabove.

In some embodiments, the at least one additional inner partition wallcomprises a plurality of additional inner partition walls such thatgreater than about 50 percent or greater than about 70 percent of theinner partition walls of the structural catalyst body comprise one ormore gradients of catalytic material described herein. In someembodiments, greater than about 90 percent of the inner partition wallsof the structural catalyst body comprise one or more gradients ofcatalytic material described herein. In some embodiments, greater thanabout 95 percent of the inner partition walls of the structural catalystbody comprise one or more gradients of catalytic material describedherein.

FIG. 2 illustrates a honeycomb-like structural catalyst body accordingto one embodiment described herein. The structural catalyst body of FIG.2 comprises an outer peripheral wall (10) and a plurality of innerpartition walls (11), wherein one or more of the inner partition walls(11) have one or more gradients of first and/or second catalyticmaterial as described herein. The inner partition walls (11) define aplurality of flow channels or cells (12) which extend longitudinallythrough the honeycomb-like structural catalyst body.

FIG. 3 illustrates a cross-section of a portion of a honeycomb-likestructural catalyst body according to one embodiment described herein.The flow channels (12) of the structural catalyst body are defined bythe inner partition walls (11). The inner partition walls (11) and theirjunctures with the outer peripheral wall (10) serve as boundaries ofadjacent flow channels (12). An inner partition wall (11) comprises afirst surface (14), a second surface (15) and a cross-sectional region(16) bridging the first surface (14) and the second surface (15). Thefirst surface (14) and/or the second surface (15) have a gradient offirst catalytic material and/or second catalytic material along thewidth of the first surface and/or the second surface as describedherein. The width of an inner partition wall surface in the embodimentof FIG. 3 is illustrated as (18). As the cross-sectional profile of flowchannels (12) of the honeycomb-like structural catalyst body illustratedin FIG. 3 is square, the inner partition walls (11) have equal orsubstantially equal widths (18).

In some embodiments, cross-sectional profiles of flow channels can benominally polygonal such as triangular, square, rectangular orhexagonal. In some embodiments, cross-sectional profiles of flowchannels can be round or oval or combinations with polygonal and curvedshapes such as annular sectors. Moreover, in some embodiments, thecross-sectional profile of the outer perimeter of the outer peripheralwall of the catalytic body can be square, rectangular, round, oval,circular sectors such as pie slices or quadrants, or any other geometricshape or shapes convenient for a given application.

FIG. 6 illustrates a cross-section of a portion of a corrugatedstructural catalyst body according to one embodiment described herein.The flow channels (61) of the structural catalyst body (60) are definedby inner partition walls (62, 63). The inner partition walls (62, 63)and their junctures or intersections with one another serve asboundaries for adjacent flow channels (61). As illustrated in FIG. 6,the corrugated catalyst body (60) comprises flat inner partition walls(63) having a width as defined by the distance between A and C. Thecorrugated catalyst body also has curved inner partition walls (62)having a width defined by the distance between A and B. Inner partitionwalls (62, 63) comprise a first surface (64) and a second surface (65).The first surface (64) and/or the second surface (65) have a gradient offirst catalytic material and/or second catalytic material along thewidth of the first surface and/or second surface as described herein.Moreover, intersection of inner partition walls (62) with one another atpoints A, B and C, for example, provide centerpost structures (66).

In some embodiments wherein the outer peripheral wall comprises a bulkfirst catalytic material, inner partition walls of a structural catalystbody comprise more bulk first catalytic material than the outerperipheral wall. In some embodiments, for example, the concentration ofbulk first catalytic material at a point in an inner partition wall isabout 1.1 to about 10 times greater than the concentration of bulk firstcatalytic material at a point in an outer peripheral wall.

In some embodiments wherein the outer peripheral wall further comprisesa bulk second catalytic material, inner partition walls of a structuralcatalyst body comprise more bulk second catalytic material than theouter peripheral wall. In some embodiments, for example, theconcentration of bulk second catalytic material at a point in an innerpartition wall is about 1.1 to about 10 times greater than theconcentration of bulk second catalytic material at a point in an outerperipheral wall.

In some embodiments, a structural catalyst body described hereincomprises a containment structure in which the inner partition walls aredisposed, such as in the arrangement of plate catalyst elements orcorrugated catalyst elements in the containment structure.

As illustrated in FIG. 3, the intersection of inner partition walls (11)of the honeycomb form centerpost structures (17). In some embodiments,intersection of spacer structures and/or walls of plate catalystelements of a structural catalyst body described herein form centerpoststructures. In some embodiments, intersection walls of corrugatedcatalyst elements of a structural catalyst body described herein formcenterpost structures.

A structural catalyst body, in some embodiments, further comprises agradient of bulk first catalytic material between a centerpost and leastone inner partition wall connected to the centerpost. In someembodiments, for example, the at least one inner partition wallcomprises a greater concentration of a bulk first catalytic materialthan the centerpost. In some embodiments, a structural catalyst bodydescribed herein comprises a gradient of bulk first catalytic materialbetween a centerpost and a plurality of inner partition walls connectedto the centerpost. In some embodiments, each of the inner partitionwalls connected to the centerpost comprises a greater concentration of abulk first catalytic material than the centerpost.

In some embodiments, the concentration of bulk first catalytic materialat a point in an inner partition wall is at least 1.1 times greater or1.3 times greater than the concentration of bulk first catalyticmaterial at a point in the centerpost. In some embodiments, theconcentration of bulk first catalytic material at a point in an innerpartition wall is at least 1.5 times or at least 2 times greater thanthe concentration of bulk first catalytic material at a point in thecenterpost. In some embodiments, the concentration of bulk firstcatalytic material at a point in an inner partition wall is at least 3times or at least 3.5 times greater than the concentration of bulk firstcatalytic material at a point in the centerpost. In some embodiments,the concentration of bulk first catalytic material at a point in aninner partition wall is at least 4 times or at least 4.5 times greaterthan the concentration of bulk first catalytic material at a point inthe centerpost. In some embodiments, the concentration of bulk firstcatalytic material at a point in an inner partition wall is at least 5times or at least 10 times greater than the concentration of bulk firstcatalytic material at a point in the centerpost. In some embodiments, aconcentration of bulk first catalytic material at a plurality of pointsin an inner partition wall is at least 1.1 times greater or 1.3 timesgreater than the concentration of bulk first catalytic material at oneor more points in the centerpost.

In some embodiments, the concentration of bulk first catalytic materialat a point in an inner partition wall is 1.3 times to 10 times greaterthan the concentration of bulk first catalytic material at a point inthe centerpost. In some embodiments, a concentration of bulk firstcatalytic material at a plurality of points in an inner partition wallis 1.3 times to 10 times greater than the concentration of bulk firstcatalytic material at one or more points in the centerpost.

A structural catalyst body, in some embodiments, further comprises agradient of bulk second catalytic material between a centerpost andleast one inner partition wall connected to the centerpost. In someembodiments, for example, the at least one inner partition wallcomprises a greater concentration of a bulk second catalytic materialthan the centerpost. In some embodiments, a structural catalyst bodydescribed herein comprises a gradient of bulk second catalytic materialbetween a centerpost and a plurality of inner partition walls connectedto the centerpost. In some embodiments, each of the inner partitionwalls connected to the centerpost comprises a greater concentration of abulk second catalytic material than the centerpost.

In some embodiments, the concentration of bulk second catalytic materialat a point in an inner partition wall is at least 1.1 times greater or1.3 times greater than the concentration of bulk second catalyticmaterial at a point in the centerpost. In some embodiments, theconcentration of bulk second catalytic material at a point in an innerpartition wall is at least 1.5 times or at least 2 times greater thanthe concentration of bulk second catalytic material at a point in thecenterpost. In some embodiments, the concentration of bulk secondcatalytic material at a point in an inner partition wall is at least 3times or at least 3.5 times greater than the concentration of bulksecond catalytic material at a point in the centerpost. In someembodiments, the concentration of bulk second catalytic material at apoint in an inner partition wall is at least 4 times or at least 4.5times greater than the concentration of bulk second catalytic materialat a point in the centerpost. In some embodiments, the concentration ofbulk second catalytic material at a point in an inner partition wall isat least 5 times or at least 10 times greater than the concentration ofbulk second catalytic material at a point in the centerpost. In someembodiments, a concentration of bulk second catalytic material at aplurality of points in an inner partition wall is at least 1.1 timesgreater or 1.3 times greater than the concentration of bulk secondcatalytic material at one or more points in the centerpost.

In some embodiments, the concentration of bulk second catalytic materialat a point in an inner partition wall is 1.3 times to 10 times greaterthan the concentration of bulk second catalytic material at a point inthe centerpost. In some embodiments, a concentration of bulk secondcatalytic material at a plurality of points in an inner partition wallis 1.3 times to 10 times greater than the concentration of bulk secondcatalytic material at one or more points in the centerpost.

Embodiments described herein contemplate structural catalyst bodieshaving any combination of the foregoing gradients of first catalyticmaterial and/or second catalytic material. In some embodiments, forexample, a structural catalyst described herein can have any combinationof gradients of first catalytic material and/or second catalyticmaterial as provided in Table I of FIG. 5.

In some embodiments, the outer peripheral wall and the inner partitionwalls of a structural catalyst body described herein are formed from asupport material such as an inorganic oxide composition, includingrefractory metal oxide compositions. The inorganic oxide composition, insome embodiments, comprises titania (TiO₂), alumina (Al₂O₃), zirconia(ZrO₂), silica (SiO₂), silicate or mixtures thereof. In someembodiments, the chemical composition comprises an inorganic oxidecomposition of TiO₂, Al₂O₃, ZrO₂ or SiO₂ or mixtures thereof in anamount ranging from about 70 weight percent to 100 weight percent. Insome embodiments, the inorganic oxide composition is sintered orotherwise heat treated to increase the mechanical integrity of thestructural catalyst body.

In some embodiments, an outer peripheral wall and the inner partitionwalls of a structural catalyst body described herein are formed from acomposition comprising catalytic material. In some embodiments, theouter peripheral wall and the inner partition walls of a structuralcatalyst body are formed of a chemical composition comprising 50-99.99%by weight an inorganic oxide composition and at least 0.01% by weight acatalytically active metal functional group. In some embodiments, thecatalytically active metal functional group can comprise any of thecatalytic materials described herein. In some embodiments, structuralcatalyst bodies comprising an outer peripheral wall and inner partitionwalls formed from a composition comprising catalytic material aredescribed in U.S. Pat. Nos. 7,807,110, 7,776,786 and 7,658,898 which arehereby incorporated by reference in their entireties. In someembodiments, the catalytically active metal functional group isdispersed throughout the chemical composition. In some embodiments, thecatalytically active metal functional group is dispersed uniformly orsubstantially uniformly throughout the chemical composition.

In some embodiments, structural catalyst bodies described hereincomprise virgin structural catalyst bodies. A virgin structural catalystbody, in some embodiments, has not been used or previously installedinto a catalytic reactor for conducting catalytic reactions in a fluidstream.

In some embodiments, a structural catalyst body described is used orregenerated. A used structural catalyst body, in some embodiments, hasbeen previously installed in a catalytic reactor for conductingcatalytic reactions in a fluid stream.

In some embodiments, catalytic material of gradients of structuralcatalyst bodies described herein comprise one or more transition metals.In some embodiments, transition metals of catalytic material comprisevanadium, tungsten, molybdenum, platinum, palladium, ruthenium, rhodium,rhenium, iron, gold, silver, copper or nickel or alloys or oxidesthereof. In some embodiments, one or more catalytic materials ofgradients of structural catalyst bodies described herein are suitablefor SCR applications and processes. In some embodiments, for example,catalytic material comprises V₂O₅, WO₃ or MoO₃ or mixtures thereof.

In some embodiments, the first catalytic material described hereincomprises a transition metal selected from the group consisting ofvanadium, tungsten, molybdenum, platinum, palladium, ruthenium, rhodium,rhenium, iron, gold, silver, copper and nickel and alloys and oxidesthereof. In some embodiments, for example, the first catalytic materialis V₂O₅, WO₃ or MoO₃. Moreover, in some embodiments, the secondcatalytic material described herein comprises a transition metalselected from the group consisting of vanadium, tungsten, molybdenum,platinum, palladium, ruthenium, rhodium, rhenium, iron, gold, silver,copper and nickel and alloys and oxides thereof. In some embodiments,for example, the second catalytic material is V₂O₅, WO₃ or MoO₃. In someembodiments, the at least one additional catalytic material describedherein comprises a transition metal selected from the group consistingof vanadium, tungsten, molybdenum, platinum, palladium, ruthenium,rhodium, rhenium, iron, gold, silver, copper and nickel and alloys andoxides thereof. In some embodiments, for example, the at least oneadditional catalytic material is V₂O₅, WO₃ or MoO₃.

Structural catalyst bodies described herein can have any dimensions andmechanical properties not inconsistent with the objectives of thepresent invention. In some embodiments, structural catalyst bodies havedimensions and mechanical properties suitable for use in SCRapplications and processes. In some embodiments, for example, structuralcatalyst bodies can have one or more properties consistent with astructural catalyst body described in U.S. Pat. Nos. 7,807,110,7,776,786 and 7,658,898. In some embodiments, structural catalyst bodiesdescribed herein comprise plate catalyst bodies or corrugated catalystbodies. In some embodiments, a structural catalyst body described hereincan comprise one or more plate catalyst element or corrugated catalystelements.

In another aspect, a catalyst module is described herein comprising aframework and a plurality of structural catalyst bodies disposed in theframework, the structural catalyst bodies comprising a gradient of firstcatalytic material along a width of a surface of at least one innerpartition wall as described herein, wherein the catalytic activity ofthe catalyst bodies of the module is substantially uniform. In beingsubstantially uniform, catalytic activity between catalyst bodies of themodule, in some embodiments, varies less than about 20%. In someembodiments, in being substantially uniform, catalytic activity betweencatalyst bodies of the module varies less than 10%. In some embodiments,in being substantially uniform, catalytic activity between catalystbodies of the module varies less than 5%. In some embodiments, catalyticactivity comprises the selective catalytic reduction of nitrogen oxides,the oxidation of mercury or the oxidation of ammonia or combinationsthereof.

In some embodiments, sulfur dioxide oxidation activity of catalystbodies of the module is substantially uniform. In being substantiallyuniform, sulfur dioxide oxidation activity between catalyst bodies ofthe module, in some embodiments, varies less than 40%. In someembodiments, in being substantially uniform, sulfur dioxide oxidationactivity between catalyst bodies of the module varies less than 20%. Insome embodiments, in being substantially uniform, sulfur dioxideoxidation activity between catalyst bodies of the module varies lessthan 10%.

Moreover, in some embodiments, catalyst bodies of a module comprise oneor more catalytic gradients described herein in addition to a gradientof a first catalytic material along the width of a surface of at leastone inner partition wall. In some embodiments, for example, catalystbodies of the module also comprise a gradient of bulk first catalyticmaterial along a width and/or length of at least one inner partition asdescribed herein. In some embodiments, catalyst bodies of a module canhave any combination of the gradients provided in Table I of FIG. 5.

In another aspect, at least one catalyst layer of a catalytic reactor isdescribed herein, the catalyst layer comprising a plurality ofstructural catalyst bodies, the structural catalyst bodies comprising agradient of first catalytic material along a width of a surface of atleast one inner partition wall as described herein, wherein thecatalytic activity of the structural catalyst bodies of the catalystlayer is substantially uniform. In being substantially uniform, in someembodiments, catalytic activity between catalyst bodies of the catalystlayer varies less than about 20%. In some embodiments, in beingsubstantially uniform, catalytic activity between catalyst bodies of thecatalyst layer varies less than about 10%. In some embodiments, in beingsubstantially uniform, catalytic activity between catalyst bodies of thecatalyst layer varies less than about 5%. In some embodiments, catalyticactivity comprises the selective catalytic reduction of nitrogen oxides,the oxidation of mercury or the oxidation of ammonia or combinationsthereof.

In some embodiments, sulfur dioxide oxidation activity of catalystbodies of the catalyst layer is substantially uniform. In beingsubstantially uniform, sulfur dioxide oxidation activity betweencatalyst bodies of the catalyst layer, in some embodiments, varies lessthan 40%. In some embodiments, in being substantially uniform, sulfurdioxide oxidation activity between catalyst bodies of the catalyst layervaries less than 20%. In some embodiments, in being substantiallyuniform, sulfur dioxide oxidation activity between catalyst bodies ofthe catalyst layer varies less than 10%.

In some embodiments, catalyst bodies of a catalyst layer comprise one ormore catalytic gradients described herein in addition to the gradient offirst catalytic material along the width of a surface of at least oneinner partition wall. In some embodiments, for example, catalyst bodiesof a catalyst layer also comprise a gradient of bulk first catalyticmaterial along a width and/or length of at least one inner partition asdescribed herein. In some embodiments, catalyst bodies of a catalystlayer can have any combination of the gradients provided in Table I ofFIG. 5.

In some embodiments, catalyst bodies of a catalyst layer are arrangedinto one or more modules.

In another aspect, methods of producing structural catalyst bodiesdescribed herein are provided. In some embodiments, a method ofproducing a structural catalyst body comprises providing a catalystsupport comprising at least one inner partition wall comprising a firstsurface and a second surface opposite the first surface, impregnatingthe at least one inner partition wall with a solution comprising a firstcatalytic material and drying the at least one inner partition wall in amanner to establish a gradient of the first catalytic material along awidth of the first surface. In some embodiments, the first catalyticmaterial of the gradient decreases in amount at the periphery of thewidth of the first surface. In some embodiments, the first catalyticmaterial of the gradient increases in amount along a central region ofthe width of the first surface.

In some embodiments, a gradient of the first catalytic material is alsoestablished along a width of the second surface. In some embodiments,the first catalytic material of the gradient decreases in amount at theperiphery of the width of the second surface. The first catalyticmaterial of the gradient, in some embodiments, increases in amount alonga central region of the width of the second surface. In someembodiments, the gradient profile of the first catalytic material alongthe width of the second surface is symmetrical or substantiallysymmetrical to the gradient profile of the first catalytic materialalong the width of the first surface.

In some embodiments, the at least one inner partition wall of thestructural catalyst support is dried in a manner to establish a gradientof bulk first catalytic material along a width of the inner partitionwall. In some embodiments, bulk first catalytic material of the gradientdecreases in concentration at the periphery of the width of the innerpartition wall. In some embodiments, bulk first catalytic materialincreases in concentration along a central region of the width of theinner partition wall. In some embodiments, a gradient of a bulk firstcatalytic material along the width of the inner partition wall has aprofile symmetrical or substantially symmetrical about the midpoint ofthe profile.

In some embodiments, the at least one inner partition wall of thestructural catalyst support is dried in a manner to establish a gradientof the first catalyst material along a length of the first surface ofthe inner partition wall. A gradient of the first catalytic materialalong the length of a first surface of the inner partition wall, in someembodiments, comprises a greater amount of the first catalytic materialat a first end of the inner partition wall in comparison with an amountof the first catalytic material at a second end of the inner partitionwall, the second end opposite the first end.

In some embodiments, a gradient of the first catalytic material is alsoestablished along a length of the second surface of the inner partitionwall. A gradient of the first catalytic material along the length of thesecond surface of the inner partition wall, in some embodiments,comprises a greater amount of the first catalytic material at a firstend of the inner partition wall in comparison with an amount of thefirst catalytic material at a second end of the inner partition wall,the second end opposite the first end. In some embodiments, the gradientprofile of the first catalytic material along the length of the secondsurface of the inner partition wall is symmetrical or substantiallysymmetrical to the gradient profile of the first catalytic materialalong the length of the first surface of the inner partition wall.

In some embodiments, the first end of the inner partition wallcorresponds to the fluid stream inlet side of the structural catalystbody and the second end corresponds to the fluid stream outlet side ofthe structural catalyst body. Alternatively, in some embodiments, thefirst end of the inner partition wall corresponds to the outlet side ofthe structural catalyst body, and the second end corresponds to thefluid stream inlet side.

In some embodiments, the at least one inner partition wall of astructural catalyst body described herein is dried in a manner toestablish a gradient of a bulk first catalytic material along a lengthof the inner partition wall. In some embodiments, a gradient of a firstbulk catalytic material along a length of the inner partition wallcomprises a greater concentration of the bulk first catalytic materialat a first end of the inner partition wall in comparison with aconcentration of the bulk first catalytic material at a second end ofthe inner partition wall, the second end opposite the first end.

In some embodiments of methods described herein, the structural catalystbody comprises a plurality of inner partition walls such that the innerpartition walls are impregnated with a solution comprising the firstcatalytic material and dried in a manner to establish a gradient of theof the first catalytic material along a width and/or length of one ormore surfaces of the inner partition walls. In some embodiments, theinner partition walls are dried in a manner to establish a gradient of abulk first catalytic material along a width and/or length of the innerpartition walls.

In some embodiments, inner partition walls of a structural catalyst bodyproduced according to methods described herein intersect to form one ormore centerposts. In some embodiments, at least one centerpost isimpregnated with a solution comprising the first catalytic material anddried in a manner to establish a gradient of bulk first catalyticmaterial between the centerpost and at least one of the inner partitionwalls. In some embodiments, for example, at least one inner partitionwall comprises a greater concentration of bulk first catalytic materialthan the centerpost. In some embodiments, each of the inner partitionwalls connected to the centerpost comprises a greater concentration ofbulk first catalytic material than the centerpost.

In some embodiments of methods described herein, the impregnatingsolution further comprises a second catalytic material. In someembodiments, a gradient of bulk metal or metal oxide second catalyticmaterial is established along a width of the inner partition wall.Alternatively, in some embodiments, at least one inner partition wall ofa structural catalyst body comprising one or more gradients of the firstcatalytic material described herein is further impregnated with asolution comprising a metal or metal oxide second catalytic material anddried in a manner to establish a gradient of the metal or metal oxidesecond catalytic material along a width of the first surface and/orsecond surface of the inner partition wall. In some embodiments, agradient of bulk metal or metal oxide second catalytic material isestablished along a width of the inner partition wall.

In some embodiments, the second catalytic material of the gradientdecreases in amount at the periphery of the width of the first surface.In some embodiments, the second catalytic material of the gradientincreases in amount along a central region of the width of the firstsurface.

In some embodiments, a gradient of the second catalytic material is alsoestablished along a width of the second surface of the inner partitionwall. In some embodiments, the second catalytic material of the gradientdecreases in amount at the periphery of the width of the second surface.The second catalytic material of the gradient, in some embodiments,increases in amount along a central region of the width of the secondsurface. In some embodiments, the gradient profile of the secondcatalytic material along the width of the second surface is symmetricalor substantially symmetrical to the gradient profile of the secondcatalytic material along the width of the first surface.

In some embodiments, a gradient of the second catalytic material is alsoestablished along a length of the first surface of the inner partitionwall. A gradient of the second catalytic material along a first surfaceof the inner partition wall, in some embodiments, comprises a greateramount of the second catalytic material at a first end of the innerpartition wall in comparison with an amount of the second catalyticmaterial at a second end of the inner partition wall, the second endopposite the first end.

In some embodiments, a gradient of the second catalytic material is alsoestablished along a length of the second surface of the inner partitionwall. A gradient of the second catalytic material along the length ofthe second surface of the inner partition wall, in some embodiments,comprises a greater amount of the second catalytic material at a firstend of the inner partition wall in comparison with an amount of thesecond catalytic material at a second end of the inner partition wall,the second end opposite the first end. In some embodiments, the gradientprofile of the second catalytic material along the length of the secondsurface of the inner partition wall is symmetrical or substantiallysymmetrical to the gradient profile of the second catalytic materialalong the length of the first surface of the inner partition wall.

In some embodiments, a gradient of bulk second catalytic material isalso established along a width of the inner partition wall. In someembodiments, bulk second catalytic material of the gradient decreases inconcentration at the periphery of the width of the inner partition wall.In some embodiments, bulk second catalytic material increases inconcentration along a central region of the width of the inner partitionwall. In some embodiments, a gradient of bulk second catalytic materialalong the width of the inner partition wall has a profile symmetrical orsubstantially symmetrical about the midpoint of the profile.

In some embodiments, drying the at least one inner partition wall of astructural catalyst body described herein also establishes a gradient ofa bulk second catalytic material along a length of the inner partitionwall. In some embodiments, a gradient of a bulk second catalyticmaterial along a length of the inner partition wall comprises a greaterconcentration of the bulk second catalytic material at a first end ofthe inner partition wall in comparison with a concentration of the bulksecond catalytic material at a second end of the inner partition wall,the second end opposite the first end.

Moreover, in some embodiments of methods described herein, a gradient ofthe second catalytic material is also established along a width and/orlength of one or more surfaces of a plurality of inner partition wallsof the structural catalyst body. In some embodiments, a gradient of bulksecond catalytic material is also established along a width and/orlength of a plurality of inner partition walls of the structuralcatalyst body.

In some embodiments, at least one centerpost of a structural catalystbody is impregnated with the solution further comprising the secondcatalytic material, and drying the structural catalyst body alsoestablishes a gradient of bulk second catalytic material between thecenterpost and at least one of the inner partition walls forming thecenterpost. In some embodiments, for example, at least one innerpartition wall comprises a greater concentration of bulk secondcatalytic material than the centerpost. In some embodiments, each of theinner partition walls forming the centerpost comprises a greaterconcentration of bulk second catalytic material than the centerpost.

Additionally, in some embodiments, the outer peripheral wall of astructural catalyst body described herein is impregnated with the secondcatalytic material. In some embodiments wherein the outer peripheralwall comprises bulk second catalytic material, inner partition walls ofthe structural catalyst body comprise a greater concentration of bulksecond catalytic material than the outer peripheral wall.

In some embodiments, first and/or second catalytic material of gradientsof structural catalyst bodies produced according to methods describedherein comprise one or more transition metals. In some embodiments,transition metals of the first and/or second catalytic material comprisevanadium, tungsten, molybdenum, platinum, palladium, ruthenium, rhodium,rhenium, iron, gold, silver, copper or nickel or alloys or oxidesthereof. In some embodiments, the first and/or second catalytic materialof gradients of structural catalyst bodies described herein are suitablefor SCR applications and processes. In some embodiments, for example,the first and/or second catalytic material comprise V₂O₅, WO₃ or MoO₃ ormixtures thereof. In some embodiments, the first and/or second catalyticmaterial comprise one or more precursors for forming a catalyticmaterial suitable for SCR applications. In some embodiments, forexample, the first and/or second catalytic material comprise one or moreprecursors for forming V₂O₅, WO₃ or MoO₃ or mixtures thereof.

In some embodiments, drying inner partition walls and/or centerposts ofa structural catalyst support comprises flowing a gas over surfaces ofthe inner partition walls and/or centerposts at a rate and/ortemperature sufficient to establish one or more gradients of the firstcatalytic material and/or second catalytic material described herein.Flowing a gas over surfaces of the inner partition walls and/orcenterposts to establish one or more gradients of the first catalyticmaterial and/or second catalytic material described herein can beadministered in any manner not inconsistent with the objectives of thepresent invention. In some embodiments, gas is flowed over all orsubstantially all of the inner partition walls and/or centerposts of astructural catalyst support in an even or substantially even manner.

Additionally, in some embodiments, the impregnation solution of a methoddescribed herein further comprises at least one additional catalyticmaterial. In such embodiments, drying the structural catalyst body canprovide one or more gradients of the additional catalytic materialhaving a construction and/or location on the structural catalyst bodyconsistent with any gradient of the first and/or second catalyticmaterial described herein.

In some embodiments, a structural catalyst support is virgin. A virginstructural catalyst support, in some embodiments, has not been used orpreviously installed into a catalytic reactor for conducting catalyticreactions in a fluid stream.

In some embodiments, a structural catalyst support is used. A usedstructural catalyst support, in some embodiments, has been previouslyinstalled in a catalytic reactor for conducting catalytic reactions in afluid stream. In some embodiments, a used catalyst support is part of astructural catalyst body in need of regeneration.

In some embodiments, virgin or used structural catalyst supportscomprise honeycomb-like structural supports, plate structural supportsor corrugated structural supports.

In some embodiments of methods described herein, structural catalystsupports comprising a plurality of inner partition walls are arranged inthe framework of a catalyst module. In such embodiments, the catalystmodule comprising the structural catalyst supports can be immersed inthe solution of catalytic material to impregnate the inner partitionwalls and/or centerposts of the structural catalyst supports withcatalytic material.

In some embodiments, the structural catalyst supports impregnated with asolution of the first catalytic material are dried while remaining theframework of the catalyst module to establish one or more gradients ofthe first catalytic material described herein. In some embodiments, theimpregnation solution further comprises a second catalytic materialwherein drying the structural catalyst supports while remaining in theframework of the catalyst module also establishes one or more gradientsof the second catalytic material as described herein. In someembodiments, for example, a gas is flowed through the module and oversurfaces of the inner partition walls and/or centerposts of thestructural catalyst supports at a rate and/or temperature sufficient toestablish one or more gradients of the first and/or second catalyticmaterial described herein. In some embodiments, the gas is flowed evenlyor substantially evenly through the structural catalyst supportsarranged in the framework of the module such that the catalytic activityof the resulting structural catalyst bodies is substantially uniformacross the module. In being substantially uniform, catalytic activitybetween catalyst bodies in the module, in some embodiments, varies lessthan about 20%. In some embodiments, in being substantially uniform,catalytic activity between catalyst bodies of the module varies lessthan 10%. In some embodiments, in being substantially uniform, catalyticactivity between catalyst bodies of the module varies less than 5%. Insome embodiments, catalytic activity comprises the selective catalyticreduction of nitrogen oxides, the oxidation of mercury or the oxidationof ammonia or combinations thereof.

In some embodiments, sulfur dioxide oxidation activity of catalystbodies of the module is substantially uniform across the module. Inbeing substantially uniform, sulfur dioxide oxidation activity betweencatalyst bodies of the module, in some embodiments, varies less than40%. In some embodiments, in being substantially uniform, sulfur dioxideoxidation activity between catalyst bodies of the module varies lessthan 20%. In some embodiments, in being substantially uniform, sulfurdioxide oxidation activity between catalyst bodies of the module variesless than 10%.

In some embodiments, gradients of first and/or second catalytic materialproduced according to the forgoing methods can have any of thestructural and/or compositional properties described herein for thegradients of the first and/or second catalytic material. In someembodiments, for example, a structural catalyst produced according toone or more methods described herein can have any combination ofgradients of first catalytic material and/or second catalytic materialas provided in Table I of FIG. 5.

In some embodiments of methods described herein, a structural catalystsupport is immersed or dipped into a solution of catalytic material toimpregnate the inner partition walls and/or centerposts with thesolution of catalytic material. In some embodiments, catalytic materialof the solution comprises one or more transition metals. In someembodiments, transition metals comprise vanadium, tungsten, molybdenum,platinum, palladium, ruthenium, rhodium, rhenium, iron, gold, silver,copper or nickel or alloys or oxides thereof. In some embodiments, oneor more catalytic materials of gradients of structural catalyst bodiesdescribed herein are suitable for SCR applications and processes. Insome embodiments, for example, catalytic material comprises V₂O₅, WO₃ orMoO₃ or mixtures thereof.

In some embodiments, the first catalytic material of a solutiondescribed herein comprises a transition metal selected from the groupconsisting of vanadium, tungsten, molybdenum, platinum, palladium,ruthenium, rhodium, rhenium, iron, gold, silver, copper and nickel andalloys and oxides thereof. Moreover, in some embodiments, the secondcatalytic material of a solution described herein comprises a transitionmetal selected from the group consisting of vanadium, tungsten,molybdenum, platinum, palladium, ruthenium, rhodium, rhenium, iron,gold, silver, copper and nickel and alloys and oxides thereof. In someembodiments, the at least one additional catalytic material of asolution described herein comprises a transition metal selected from thegroup consisting of vanadium, tungsten, molybdenum, platinum, palladium,ruthenium, rhodium, rhenium, iron, gold, silver, copper and nickel andalloys and oxides thereof.

In some embodiments, for example, an aqueous solution comprises firstcatalytic material of a vanadium salt, such as vanadyl salts, includingvanadyl oxalate, vanadyl sulfate or ammonium metavanadate or mixturesthereof. In some embodiments, the aqueous solution further comprises asecond catalytic material of a tungsten salt, such as tungstate salts,including ammonium metatungstate. In some embodiments, the aqueoussolution further comprises at least one additional catalytic material ofa molybdenum salt, such as ammonium molybdate, sodium molybdate ormixtures thereof.

A catalytic material can be present in a solution for impregnating thecatalyst support in any amount not inconsistent with the objectives ofthe present invention.

In some embodiments, a structural catalyst support is immersed in asolution of the first, second and/or additional catalytic material forany desired amount of time not inconsistent with the objectives of thepresent invention. In some embodiments, a structural catalyst support isimmersed in a solution of catalytic material for a time period of atleast about 5 seconds. In some embodiments, a structural catalystsupport is immersed in a solution of catalytic material for a timeperiod of at least about 10 seconds or at least about 30 seconds. Insome embodiments, a structural catalyst support is immersed in asolution of catalytic material for a time period of at least about 1minute. In some embodiments, a structural catalyst support is immersedin a solution of catalytic material for a time period of at least about5 minutes or at least about 10 minutes. A structural catalyst support,in some embodiments, is immersed in a solution of catalytic material fora time period ranging from about 1 minute to about 15 minutes.

In some embodiments, pore surfaces and/or other surfaces of a structuralcatalyst support are not treated with a blocking fluid or other agenthaving the ability to inhibit or facilitate impregnation of the solutionof catalytic material into the inner partition walls and/or centerpostsprior or subsequent to immersing the structural catalyst body in thesolution of catalytic material.

In some embodiments, a structural catalyst support is fully immersed inthe solution of catalytic material. In some embodiments, a catalystsupport is only partially immersed in the solution of catalyticmaterial.

Moreover, in some embodiments of methods described herein, structuralcatalyst supports comprising a plurality of inner partition walls arearranged in the framework of a catalyst module. In such embodiments, thecatalyst module comprising the structural catalyst supports can beimmersed in the solution of the first, second and/or additionalcatalytic material to impregnate the inner partition walls and/orcenterposts of the structural catalyst supports with catalytic material.

Inner partition walls and/or centerposts of a structural catalystsupport are dried to establish one or more gradients of the first,second and/or additional catalytic material described herein. In someembodiments, drying inner partition walls and/or centerposts of astructural catalyst support comprises flowing a gas over surfaces of theinner partition walls and/or centerposts at a rate and/or temperaturesufficient to establish one or more of the gradients of catalyticmaterial described herein.

A gas flowed over surfaces of the inner partition walls and/orcenterposts of a structural catalyst support during the drying processcan have any desired flow rate consistent with establishing one or moregradients of catalytic material described herein. In some embodiments, agas has a flow rate according to any of the ranges set forth in Table I.

TABLE I Drying Gas Flow Rate (m/s) 0.1-1   1-2 2-3 3-4 4-5 5-6 6-7 7-88-9  9-10 >10

Moreover, a gas flowed over surfaces of the inner partition walls and/orcenterposts of a structural catalyst support during the drying processcan have any desired temperature consistent with establishing one ormore gradients of catalytic material described herein. The gas, in someembodiments, is heated to a temperature of at least about 140° C. Insome embodiments, the gas is heated to a temperature of at least about160° C. In some embodiments, the gas is heated to a temperature rangingfrom about 100° C. to about 350° C. In some embodiments, the gas isheated to a temperature greater than 350° C.

In some embodiments, the flow rate of the gas and the temperature of thegas can be mutually or independently adjusted to produce gradients ofcatalytic material of varying degree along widths of inner partitionwalls of a structural catalyst support in the production of a structuralcatalyst body.

A gas suitable for flowing over surfaces of one or more inner partitionwalls can comprise any gas not inconsistent with establishing one ormore gradients of catalytic material described herein. In someembodiments, a gas comprises air. In some embodiments, a gas comprisesnitrogen or argon. In some embodiments, a gas comprises combustion fluegas. In some embodiments, a structural catalyst body described herein iscalcined after establishing one or more gradients of catalytic material.

Inner partition walls and/or centerposts of a structural catalystsupport can be exposed to the flowing gas for any desired time periodconsistent with establishing one or more gradients of catalytic materialdescribed herein. In some embodiments, inner partition walls and/orcenterposts are exposed to the flowing gas for a time period rangingfrom about 1 minute to about 1.5 hours. In some embodiments, innerpartition walls and/or centerposts are exposed to the flowing gas for atime period ranging from about 5 minutes to about 45 minutes. In someembodiments, inner partition walls and/or centerposts are exposed to theflowing gas for a time period ranging from about 10 minutes to about 30minutes.

Flowing a gas over surfaces of the inner partition walls and/orcenterposts to establish one or more gradients of catalytic materialdescribed herein can be administered in any manner not inconsistent withthe objectives of the present invention. In some embodiments, gas isflowed over all or substantially all of the inner partition walls and/orcenterposts of a structural catalyst support in an even or substantiallyeven manner. In some embodiments, for example, a conduit is coupled tothe open face of the catalyst support, and gas is flowed through theconduit and through the flow channels of the structural catalystsupport, thereby flowing evenly or substantially evenly over the innerpartition walls and/or centerposts. In some embodiments, the conduit issealed to the open face of the structural catalyst support or precludeor inhibit air flow along exterior surfaces of the structural catalystsupport.

In some embodiments, a diffuser is positioned in front of the open faceof the catalyst support to assist in providing an even or substantiallyeven flow of the gas through the structural catalyst body during thedrying process. In some embodiments, a diffuser can comprise aperforated plate. Additionally, in some embodiments, a diffuser can beused alone or in conjunction with a conduit.

In some embodiments, the structural catalyst supports impregnated with asolution of the first, second and/or additional catalytic material aredried while remaining the framework of the catalyst module to establishone or more gradients of catalytic material described herein. In someembodiments, for example, a gas is flowed through the module and oversurfaces of the inner partition walls and/or centerposts of thestructural catalyst supports at a rate and/or temperature sufficient toestablish one or more gradients of catalytic material described herein.

In some embodiments, the gas is flowed evenly or substantially evenlythrough the structural catalyst supports arranged in the framework ofthe module such that the catalytic activity of the resulting structuralcatalyst bodies is substantially uniform across the module. In beingsubstantially uniform, catalytic activity between catalyst bodies in themodule, in some embodiments, varies less than about 20%. In someembodiments, in being substantially uniform, catalytic activity betweencatalyst bodies of the module varies less than 10%. In some embodiments,in being substantially uniform, catalytic activity between catalystbodies of the module varies less than 5%. In some embodiments, catalyticactivity comprises the selective catalytic reduction of nitrogen oxides,the oxidation of mercury or the oxidation of ammonia or combinationsthereof.

In some embodiments, sulfur dioxide oxidation activity of catalystbodies of the module is substantially uniform across the module. Inbeing substantially uniform, sulfur dioxide oxidation activity betweencatalyst bodies of the module, in some embodiments, varies less than40%. In some embodiments, in being substantially uniform, sulfur dioxideoxidation activity between catalyst bodies of the module varies lessthan 20%. In some embodiments, in being substantially uniform, sulfurdioxide oxidation activity between catalyst bodies of the module variesless than 10%.

In some embodiments, a conduit is coupled to the open face of the moduleand gas is flowed through the conduit and through the structuralcatalyst supports in the module. In some embodiments, the conduit issealed to the open face of the module to preclude or inhibit air flowalong exterior surfaces of the module.

In some embodiments, a diffuser is positioned in front of the open faceof the catalyst module to assist in providing an even or substantiallyeven flow of the gas through the structural catalyst body during thedrying process. In some embodiments, a diffuser can comprise aperforated plate. Additionally, in some embodiments, a diffuser can beused alone or in conjunction with a conduit.

In another aspect, methods of treating a fluid stream, such as a fluegas or combustion gas stream are described herein. In some embodiments,a method of treating a fluid stream comprises providing a structuralcatalyst body comprising at least one inner partition wall comprising afirst surface and a second surface opposite the first surface, the innerpartition wall having a gradient of first catalytic material along awidth of the first surface, passing the fluid stream through thestructural catalyst body and catalytically reacting at least onechemical species in the fluid stream. In some embodiments, the fluidstream is flowed through one or more flow channels of the structuralcatalyst body.

In some embodiments, catalytically reacting at least one chemicalspecies in the fluid stream comprises catalytically reducing nitrogenoxides in the fluid stream. In some embodiments, catalytically reactingat least one chemical species in the fluid stream comprises oxidizingammonia and/or mercury in the fluid stream.

In some embodiments of methods of treating a fluid stream, oxidation ofsulfur dioxide to sulfur trioxide in the fluid stream is reduced. In oneembodiment, for example, oxidation of sulfur dioxide is reduced duringthe selective catalytic reduction of nitrogen oxides in a fluid streamby a structural catalyst body described herein.

In some embodiments, catalyst bodies of a method of treating a fluidstream comprise one or more catalytic gradients described herein inaddition to the gradient of first catalytic material along the width ofa surface of at least one inner partition wall. In some embodiments, forexample, catalyst bodies also comprise a gradient of bulk firstcatalytic material along a width and/or length of at least one innerpartition as described herein. In some embodiments, catalyst bodies ofmethods described herein can have any combination of the gradientsprovided in Table I of FIG. 5.

In some embodiments, the catalyst body is part of a module comprising aplurality of catalyst bodies described herein, where the fluid stream ispassed into the module and through the catalyst bodies. In someembodiments, the module is part of a catalytic layer of a catalyticreactor.

These and other embodiments of structural catalyst bodies are furtherillustrated by the following non-limiting example.

Example 1 Structural Catalyst Body

An extrusion composition was provided by mixing TiO₂ powders withfillers, binders, extrusion aids and lubricants. The extrusioncomposition contained substantially no vanadium (<0.10% V₂O₅). Theextrusion composition included a tungsten content of ≦1.80% WO₃. Theextrusion composition was extruded to provide a structural catalystsupport comprising an outer peripheral wall and a plurality of innerpartition walls. The inner partition walls defined a plurality of flowchannels of the structural catalyst support, the flow channels having asquare cross-sectional profile. The extruded catalyst support was driedand calcined. Porosity of the structural catalyst support was determinedby a water absorption test.

A solution of a vanadium first catalytic material and a tungsten secondcatalytic material was provided by adding vanadyl oxalate solution andammonium metatungstate powder to a container of deionized water. Asunderstood by one of skill in the art, the amounts of vanadyl oxalateand ammonium metatungstate added were determined according to thedesired bulk chemistry and porosity of the structural catalyst support.Solution concentration of catalytic material was confirmed by x-rayfluorescence (XRF). The structural catalyst body was immersed in thecatalytic material solution for three minutes and subsequently removed.

The structural catalyst support impregnated with vanadium firstcatalytic material and tungsten second catalytic material was dried witha hot air blower. The structural catalyst body was wrapped and sealed ina manner such that heated air received from the blower flowed throughthe flow channels and over the inner partition walls in a substantiallyeven manner. As described herein, a conduit can be sealed to the face ofthe structural catalyst body for delivery of the heated air. The airfrom the blower was heated at a rate of 20° C./min to a set pointtemperature of 160° C. and held for 30 minutes to dry the structuralcatalyst body. The temperature of the air was then increased to 350° C.at a rate of 20° C./min to administer a 15 minute calcination of thestructural catalyst body. The resulting structural catalyst bodydemonstrated a gradient of first (V₂O₅) and second (WO₃) catalyticmaterials consistent with that illustrated in FIG. 1.

Moreover, the catalytic activity of structural catalyst bodies producedin accordance with this example for the selective catalytic reduction ofnitrogen oxides and sulfur dioxide oxidation was measured. The catalyticactivity of the structural catalyst bodies was compared to a priorstructural catalyst bodies lacking gradients of first and secondcatalytic material along widths of the inner partition walls. FIG. 4illustrates the results of the catalytic activity testing. Asillustrated in FIG. 4, the structural catalyst bodies of the presentexample (A) demonstrated significantly higher rate for the selectivereduction of nitrogen oxides per unit of sulfur dioxide oxidation incomparison to the prior catalyst bodies (B).

Various embodiments of the invention have been described in fulfillmentof the various objects of the invention. It should be recognized thatthese embodiments are merely illustrative of the principles of thepresent invention. Numerous modifications and adaptations thereof willbe readily apparent to those skilled in the art without departing fromthe spirit and scope of the invention.

1. A structural catalyst body comprising: at least one inner partitionwall comprising a first surface and a second surface opposite the firstsurface, the inner partition wall having a gradient of a first catalyticmaterial along a width of the first surface.
 2. The structural catalystbody of claim 1, wherein the first catalytic material of the gradientdecreases in amount at the periphery of the width of the first surface.3. The structural catalyst body of claim 1, wherein the first catalyticmaterial of the gradient increases in amount along a central region ofthe width of the first surface.
 4. The structural catalyst body of claim1, wherein the gradient of the first catalytic material has a profilesubstantially symmetrical about a midpoint of the profile.
 5. Thestructural catalyst body of claim 3, wherein the amount of the firstcatalytic material at a point in the central region of the width of thefirst surface is at least 1.3 times greater than an amount of the firstcatalytic material at a peripheral point of the width of the firstsurface.
 6. The structural catalyst body of claim 3, wherein the amountof the first catalytic material at a point in the central region of thewidth of the first surface is at least 2 times greater than an amount ofthe first catalytic material at a peripheral point of the width of thefirst surface.
 7. The structural catalyst body of claim 1, wherein thestructural catalyst body further comprises a gradient of the firstcatalytic material along a width of the second surface.
 8. Thestructural catalyst body of claim 7, wherein the first catalyticmaterial of the gradient decreases in amount at the periphery of thewidth of the second surface.
 9. The structural catalyst body of claim 7,wherein the first catalytic material of the gradient increases in amountalong a central region of the width of the second surface.
 10. Thestructural catalyst body of claim 7, wherein the gradient of the firstcatalytic material along the second surface is substantially symmetricalto the gradient of the first catalytic material along the first surface.11. The structural catalyst body of claim 1 further comprising agradient of a second catalytic material along the width of the firstsurface.
 12. The structural catalyst body of claim 11, wherein thesecond catalytic material of the gradient decreases in amount at theperiphery of the width of the first surface.
 13. The structural catalystbody of claim 11, wherein the second catalytic material of the gradientincreases in amount along a central region of the width of the firstsurface.
 14. The structural catalyst body of claim 13, wherein theamount of the second catalytic material at a point in the central regionof the width of the first surface is at least 1.3 times greater than anamount of the second catalytic material at a peripheral point of thewidth of the first surface.
 15. The structural catalyst body of claim11, wherein the structural catalyst body further comprises a gradient ofthe second catalytic material along a width of the second surface. 16.The structural catalyst body of claim 15, wherein the second catalyticmaterial of the gradient increases in amount along a central region ofthe width of the second surface.
 17. The structural catalyst body ofclaim 16, wherein the amount of the second catalytic material at a pointin the central region of the width of the second surface is at least 1.3times greater than an amount of the second catalytic material at aperipheral point of the width of the second surface.
 18. The structuralcatalyst body of claim 1 further comprising a gradient of the firstcatalytic material along a length of the first surface, wherein agreater amount of the first catalytic material is present at a first endof the structural catalyst body in comparison with an amount of thefirst catalytic material at a second end of the structural catalystbody, the second end opposite the first end.
 19. The structural catalystbody of claim 18, wherein the first end corresponds to the fluid streaminlet side of the structural catalyst body.
 20. The structural catalystbody of claim 18 further comprising a gradient of a second catalyticmaterial along the length of the first surface, wherein a greater amountof the second catalytic material is present at the first end of thestructural catalyst body in comparison with an amount of the secondcatalytic material at the second end of the structural catalyst body.21. The structural catalyst body of claim 18 further comprising agradient of the first catalytic material along the length of the secondsurface, wherein a greater amount of the first catalytic material ispresent at the first end of the structural catalyst body in comparisonwith an amount of the first catalytic material at the second end of thestructural catalyst body.
 22. The structural catalyst body of claim 21further comprising a gradient of a second catalytic material along thelength of the second surface, wherein a greater amount of the secondcatalytic material is present at the first end of the structuralcatalyst body in comparison with an amount of the second catalyticmaterial at a second end of the structural catalyst body.
 23. Thestructural catalyst body of claim 1, further comprising a plurality ofadditional inner partition walls comprising a first surface and a secondsurface opposite the first surface, the additional inner partition wallshaving a gradient of the first catalytic material along a width of thefirst surface, the first catalytic material increasing in amount along acentral region of the width of the first surface wherein the amount ofthe first catalytic material at a point in the central region is atleast 1.3 times greater than an amount of the first catalytic materialat a peripheral point of the width of the first surface.
 24. Thestructural catalyst body of claim 23, wherein greater than 50 percent ofthe inner partition walls of the structural catalyst body comprise thegradient of the first catalytic material along a width of the firstsurface.
 25. The structural catalyst body of claim 23, wherein greaterthan 90 percent of the inner partition walls of the structural catalystbody comprise the gradient of the first catalytic material along a widthof the first surface.
 26. The structural catalyst body of claim 24,wherein the first catalytic material is operable for the selectivecatalytic reduction of nitrogen oxides.
 27. The structural catalyst bodyof claim 24, wherein the first catalytic material is selected from thegroup consisting of V₂O₅, WO₃, MoO₃ and Ru.
 28. The structural catalystbody of claim 11, further comprising a plurality of additional innerpartition walls comprising a first surface and a second surface oppositethe first surface, the additional inner partition walls having agradient of the second catalytic material along a width of the firstsurface, the second catalytic material increasing in amount along acentral region of the width of the first surface wherein the amount ofsecond catalytic material at a point in the central region is at least1.3 times greater than an amount of the second catalytic material at aperipheral point of the width of the first surface.
 29. The structuralcatalyst body of claim 28, wherein the second catalytic material isoperable for the selective catalytic reduction of nitrogen oxides. 30.The structural catalyst body of claim 28, wherein the second catalyticmaterial is selected from the group consisting of V₂O₅, WO₃, MoO₃ andRu.
 31. A structural catalyst body comprising: at least one innerpartition wall comprising a gradient of a bulk first catalytic materialalong a width of the inner partition wall.
 32. The structural catalystbody of claim 31, wherein the bulk first catalytic material of thegradient decreases in concentration at the periphery of the width of theinner partition wall.
 33. The structural catalyst body of claim 31,wherein the bulk first catalytic material of the gradient increases inconcentration along a central region of the width of the inner partitionwall.
 34. The structural catalyst body of claim 31, wherein the gradientof the bulk first catalytic material has a profile substantiallysymmetrical about a midpoint of the profile.
 35. The structural catalystbody of claim 33, wherein the concentration of the bulk first catalyticmaterial at a point in the central region of the width of the innerpartition wall is at least 1.3 times greater than a concentration of thebulk first catalytic material at a peripheral point of the width of thefirst surface.
 36. The structural catalyst body of claim 33, wherein theconcentration of bulk first catalytic material at a point in the centralregion of the width of the inner partition wall is at least 2 timesgreater than a concentration of the bulk first catalytic material at aperipheral point of the width of the first surface.
 37. The structuralcatalyst body of claim 31 further comprising a gradient of a bulk secondcatalytic material along a width of the inner partition wall.
 38. Thestructural catalyst body of claim 37, wherein the bulk second catalyticmaterial of the gradient decreases in concentration at the periphery ofthe width of the inner partition wall.
 39. The structural catalyst bodyof claim 37, wherein the bulk second catalytic material of the gradientincreases in concentration along a central region of the width of theinner partition wall.
 40. The structural catalyst body of claim 31,further comprising a plurality of additional inner partition wallscomprising a gradient of bulk first catalytic material along a width ofthe inner partition walls, the bulk first catalytic material increasingin concentration along a central region of the width of the innerpartition walls wherein the concentration of the bulk first catalyticmaterial at a point in the central region is at least 1.3 times greaterthan a concentration of the bulk first catalytic material at aperipheral point of the width of the inner partition walls.
 41. Thestructural catalyst body of claim 40, wherein the bulk first catalyticmaterial is operable for the selective catalytic reduction of nitrogenoxides.
 42. The structural catalyst body of claim 40, wherein the bulkfirst catalytic material is selected from the group consisting of V₂O₅,WO₃, MoO₃ and Ru.
 43. The structural catalyst body of claim 40, furthercomprising a gradient of bulk second catalytic material along the widthof the inner partition walls, the bulk second catalytic materialincreasing in concentration along the central region of the width of theinner partition walls wherein the concentration of the bulk secondcatalytic material at a point in the central region is at least 1.3times greater than a concentration of the bulk second catalytic materialat a peripheral point of the width of the inner partition walls.
 44. Thestructural catalyst body of claim 43, wherein the bulk second catalyticmaterial is operable for the selective catalytic reduction of nitrogenoxides.
 45. The structural catalyst body of claim 43, wherein the bulksecond catalytic material is selected from the group consisting of V₂O₅,WO₃, MoO₃ and Ru.
 46. The structural catalyst body of claim 40, whereingreater than 50 percent of the inner partition walls of the structuralcatalyst body comprise the gradient of the bulk first catalyticmaterial.
 47. The structural catalyst body of claim 40, wherein greaterthan 90 percent of the inner partition walls of the structural catalystbody comprise the gradient of the bulk first catalytic material.
 48. Astructural catalyst body comprising: a plurality of inner partitionwalls intersecting to form a plurality of centerposts, wherein at leastone of the centerposts comprises a concentration of bulk first catalyticmaterial that is at least 1.3 times less than the concentration of bulkfirst catalytic material of each of the inner partition walls formingthe centerpost.
 49. The structural catalyst body of claim 48, whereingreater than 50% of the centerposts comprise a concentration of the bulkfirst catalytic material that is at least 1.3 times less than theconcentration of the bulk first catalytic material of each of the innerpartition walls forming the centerposts.
 50. The structural catalystbody of claim 48, wherein at least one of the centerposts comprises aconcentration of bulk second catalytic material that is at least 1.3times less than the concentration of bulk second catalytic material ofeach of the inner partition walls forming the centerpost.
 51. Thestructural catalyst body of claim 50, wherein greater than 50% of thecenterposts comprise a concentration of the bulk second catalyticmaterial that is at least 1.3 times less than the concentration of thebulk second catalytic material of each of the inner partition wallsforming the centerposts.
 52. A catalyst module comprising: a framework;and a plurality of structural catalyst bodies disposed in the framework,the structural catalyst bodies comprising a plurality of inner partitionwalls, the inner partition walls comprising a gradient of a firstcatalytic material along a width of a first surface of the innerpartition walls, the first catalytic material increasing in amount alonga central region of the width of the first surface wherein the amount ofthe first catalytic material at a point in the central region is atleast 1.3 times greater than an amount of the first catalytic materialat a peripheral point of the width of the first surface.
 53. Thecatalyst module of claim 52, wherein greater than 50% of the innerpartition walls of the structural catalyst bodies comprise the gradientof the first catalytic material.
 54. The catalyst module of claim 52,wherein the inner partition walls further comprise a gradient of asecond catalytic material along the width of the first surface.
 55. Thecatalyst module of claim 52, wherein the catalytic activity between thecatalyst bodies is substantially uniform.
 56. The catalyst module ofclaim 52, wherein catalytic activity between the catalyst bodies of themodule varies less than 10%.
 57. The catalyst module of claim 52,wherein sulfur dioxide activity between catalyst bodies of the module issubstantially uniform.
 58. The catalyst module of claim 52, whereinsulfur dioxide activity between the catalyst bodies of the module variesless than 20%.
 59. A catalyst layer comprising: a plurality ofstructural catalyst bodies, the structural catalyst bodies comprising aplurality of inner partition walls, the inner partition walls comprisinga gradient of a first catalytic material along a width of a firstsurface of the inner partition walls, the first catalytic materialincreasing in amount along a central region of the width of the firstsurface wherein the amount of the first catalytic material at a point inthe central region is at least 1.3 times greater than an amount of thefirst catalytic material at a peripheral point of the width of the firstsurface.
 60. The catalyst layer of claim 59, wherein greater than 50% ofthe inner partition walls of the structural catalyst bodies comprise thegradient of the first catalytic material.
 61. The catalyst layer ofclaim 59, wherein the inner partition walls further comprise a gradientof a second catalytic material along the width of the first surface. 62.The catalyst layer of claim 59, wherein the catalytic activity betweenthe catalyst bodies is substantially uniform.
 63. The catalyst layer ofclaim 58, wherein catalytic activity between the catalyst bodies of thelayer varies less than 10%.
 64. The catalyst layer of claim 59, whereinsulfur dioxide activity between catalyst bodies of the layer issubstantially uniform.
 65. The catalyst module of claim 59, whereinsulfur dioxide activity between the catalyst bodies of the catalystlayer varies less than 20%.
 66. A structural catalyst body comprising: aplurality of inner partition walls comprising a first surface and asecond surface opposite the first surface, wherein at least 50% of theinner partition walls comprise: a gradient of a first catalytic materialalong a width of a first surface of the inner partition walls, the firstcatalytic material increasing in amount along a central region of thewidth of the first surface wherein the amount of the first catalyticmaterial at a point in the central region is at least 1.3 times greaterthan an amount of the first catalytic material at a peripheral point ofthe width of the first surface; and a gradient of a first catalyticmaterial along a width of the second surface of the inner partitionwalls, the first catalytic material increasing in amount along a centralregion of the width of the second surface wherein the amount of thefirst catalytic material at a point in the central region is at least1.3 times greater than an amount of the first catalytic material at aperipheral point of the width of the second surface.
 67. The structuralcatalyst body of claim 66, wherein the amount of the first catalyticmaterial at a point in the central region is at least 2 times greaterthan the amount of the first catalytic material at a peripheral point ofthe width of the first surface.
 68. A structural catalyst bodycomprising: a plurality of inner partition walls comprising a firstsurface and a second surface opposite the first surface, wherein atleast 50% of the inner partition walls comprise: a gradient of a firstcatalytic material along a width of a first surface of the innerpartition walls, the first catalytic material increasing in amount alonga central region of the width of the first surface wherein the amount ofthe first catalytic material at a point in the central region is atleast 1.3 times greater than an amount of the first catalytic materialat a peripheral point of the width of the first surface; and a gradientof a first catalytic material along a width of the second surface of theinner partition walls, the first catalytic material increasing in amountalong a central region of the width of the second surface wherein theamount of the first catalytic material at a point in the central regionis at least 1.3 times greater than an amount of the first catalyticmaterial at a peripheral point of the width of the second surface; theinner partition walls intersecting to form a plurality of centerposts,wherein at least one of the centerposts comprises a concentration ofbulk first catalytic material that is at least 1.3 times less than theconcentration of bulk first catalytic material of each of the innerpartition walls forming the centerpost.
 69. The structural catalyst bodyof claim 68, wherein the amount of the first catalytic material at apoint in the central region is at least 2 times greater than the amountof the first catalytic material at a peripheral point of the width ofthe first surface.